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Manipulation of exchange bias with electric field is appealing to boost energy efficiency in spintronic devices. Here, this effect is shown at room temperature in Ir20Mn80/Fe80Ga20/Ta layers grown onto «011»-oriented PMN-32PT single crystals. After magnetic field-cooling (FC) along the [01-1] and [100] in-plane directions of PMN-32PT and upon allowing the system to relax through consecutive hysteresis loops (training effect), the exchange bias field (HEB) is measured under the action of voltage (out-of-plane poling). Depending on the applied voltage (magnitude and sign), HEB can either increase or decrease with respect to its value at 0 V. The relative variations of HEB are 24% and 5.5% after FC along the [01-1] and [100] directions, respectively. These results stem from strain-mediated magnetoelectric coupling. The applied electric field causes changes in the coercivity and the squareness ratio of the films, suggesting a reorientation of the effective magnetic easy axis in Fe80Ga20. However, larger HEB values are observed when the squareness ratio is lower. It is claimed that the effect of voltage is equivalent to an in-plane component of an applied magnetic field oriented perpendicular to the cooling field direction. Perpendicular in-plane magnetic fields have been shown to induce an increase in exchange bias in some ferromagnetic/antiferromagnetic systems due to partial recovery of the untrained antiferromagnetic state. Remarkably, here, this effect is directly induced with voltage, therefore enhancing energy efficiency.

Magneto-ionics is an emerging field in materials science where voltage is used as an energy-efficient means to tune magnetic properties, such as magnetization, coercive field, or exchange bias, by voltage-driven ion transport. We first discuss the emergence of magneto-ionics in the last decade, its core aspects, and key avenues of research. We also highlight recent progress in materials and approaches made during the past few years. We then focus on the "structural-ion"approach as developed in our research group in which the mobile ions are already present in the target material and discuss its potential advantages and challenges. Particular emphasis is given to the energetic and structural benefits of using nitrogen as the mobile ion, as well as on the unique manner in which ionic motion occurs in CoN and FeN systems. Extensions into patterned systems and textures to generate imprinted magnetic structures are also presented. Finally, we comment on the prospects and future directions of magneto-ionics and its potential for practical realizations in emerging fields, such as neuromorphic computing, magnetic random-access memory, or micro- and nano-electromechanical systems.

Magneto-ionics is an emerging actuation mechanism to control the magnetic properties of materials via voltage-driven ion motion. This effect largely relies on the strength and penetration of the induced electric field into the target material, the amount of generated ion transport pathways, and the ionic mobility inside the magnetic media. Optimizing all these factors in a simple way is a huge challenge, although highly desirable for technological applications. Here, we demonstrate that the introduction of suitable transition-metal elements to binary nitride compounds can drastically boost magneto-ionics. More specifically, we show that the attained magneto-ionic effects in CoN films (i.e., saturation magnetization, toggling speeds, and cyclability) can be drastically enhanced through 10% substitution of Co by Mn in the thin-film composition. Incorporation of Mn leads to transformation from nanocrystalline into amorphous-like structures, as well as from metallic to semiconducting behaviors, resulting in an increase of N-ion transport channels. Ab initio calculations reveal a lower energy barrier for CoMn-N compared to Co-N that provides a fundamental understanding of the crucial role of Mn addition in the voltage-driven magnetic effects. These results constitute an important step forward toward enhanced voltage control of magnetism via electric field-driven ion motion.

Magneto-ionics, which deals with the change of magnetic properties through voltage-driven ion migration, is expected to be one of the emerging technologies to develop energy-efficient spintronics. While a precise modulation of magnetism is achieved when voltage is applied, much more uncontrolled is the spontaneous evolution of magneto-ionic systems upon removing the electric stimuli (i.e., post-stimulated behavior). Here, we demonstrate a voltage-controllable N ion accumulation effect at the outer surface of CoN films adjacent to a liquid electrolyte, which allows for the control of magneto-ionic properties both during and after voltage pulse actuation (i.e., stimulated and post-stimulated behavior, respectively). This effect, which takes place when the CoN film thickness is below 50 nm and the voltage pulse frequency is at least 100 Hz, is based on the trade-off between generation (voltage ON) and partial depletion (voltage OFF) of ferromagnetism in CoN by magneto-ionics. This novel effect may open opportunities for new neuromorphic computing functions, such as post-stimulated neural learning under deep sleep.

Voltage control of magnetism via electric-field-driven ion migration (magneto-ionics) has generated intense interest due to its potential to greatly reduce heat dissipation in a wide range of information technology devices, such as magnetic memories, spintronic systems or artificial neural networks. Among other effects, oxygen ion migration in transition-metal-oxide thin films can lead to the generation or full suppression of controlled amounts of ferromagnetism ('ON-OFF' magnetic transitions) in a non-volatile and fully reversible manner. However, oxygen magneto-ionic rates at room temperature are generally considered too slow for industrial applications. Here, we demonstrate that sub-second ON-OFF transitions in electrolyte-gated paramagnetic cobalt oxide films can be achieved by drastically reducing the film thickness from >200 nm down to 5 nm. Remarkably, cumulative magneto-ionic effects can be generated by applying voltage pulses at frequencies as high as 100 Hz. Neuromorphic-like dynamic effects occur at these frequencies, including potentiation (cumulative magnetization increase), depression (i.e., partial recovery of magnetization with time), threshold activation, and spike time-dependent magnetic plasticity (learning and forgetting capabilities), mimicking many of the biological synapse functions. The systems under investigation show features that could be useful for the design of artificial neural networks whose magnetic properties would be governed with voltage.

[EN] The present invention relates to a magnetoelectric device (D), comprising: - a magnetoelectric element (Me); and - an electric voltage source (PS) configured and arranged to induce on the magnetoelectric element (Me), at least at room temperature, ON-OFF states and OFF-ON states magnetic transitions, by applying or removing determined electric voltages, wherein at said ON state the magnetoelectric element (Me) shows permanent and net magnetization. The magnetoelectric element (Me) is configured and arranged to induce the ON-OFF states and OFF-ON states magnetic transitions by means of an ion-migration mechanism and/or a piezostrain-mediated mechanism. The present invention further relates to different uses of the magnetoelectric device of the first aspect of the present invention, including a use for implementing a data security device, and uses for information and communications technologies, including neuromorphic computing and/or stochastic data storage and/or stochastic data processing., [FR] La présente invention concerne un dispositif magnétique (D), comprenant : - un élément magnétoélectrique (Me) ; et - une source de tension électrique (PS) conçue et agencée pour induire sur l'élément magnétoélectrique (Me), au moins à température ambiante, des états ACTIVATION-DÉSACTIVATION et des états DÉSACTIVATION-ACTIVATION des transitions magnétiques, par application ou suppression de tensions électriques déterminées, à l'état ACTIVATION, l'élément magnétoélectrique (Me) présentant une magnétisation permanente et nette. L'élément magnétoélectrique (Me) est conçu et agencé de façon à induire les états ACTIVATION-DÉSACTIVATION et les états DÉSACTIVATION-ACTIVATION des transitions magnétiques au moyen d'un mécanisme de migration d'ions et/ou d'un mécanisme médié par contrainte piézoélectrique. La présente invention concerne en outre différentes utilisations du dispositif magnétoélectrique du premier aspect de la présente invention, comprenant une utilisation pour mettre en œuvre un dispositif de sécurité de données, et des utilisations pour les technologies de l'information et des communications, comprenant le calcul neuromorphique et/ou le stockage de données stochastiques et/ou le traitement de données stochastiques.

Voltage control of magnetism via electric-field-driven ion migration (magneto-ionics) has generated intense interest due to its potential to greatly reduce heat dissipation in a wide range of information technology devices, such as magnetic memories, spintronic systems or artificial neural networks. Among other effects, oxygen ion migration in transition-metal-oxide thin films can lead to the generation or full suppression of controlled amounts of ferromagnetism ('ON-OFF' magnetic transitions) in a non-volatile and fully reversible manner. However, oxygen magneto-ionic rates at room temperature are generally considered too slow for industrial applications. Here, we demonstrate that sub-second ON-OFF transitions in electrolyte-gated paramagnetic cobalt oxide films can be achieved by drastically reducing the film thickness from >200 nm down to 5 nm. Remarkably, cumulative magneto-ionic effects can be generated by applying voltage pulses at frequencies as high as 100 Hz. Neuromorphic-like dynamic effects occur at these frequencies, including potentiation (cumulative magnetization increase), depression (i.e., partial recovery of magnetization with time), threshold activation, and spike time-dependent magnetic plasticity (learning and forgetting capabilities), mimicking many of the biological synapse functions. The systems under investigation show features that could be useful for the design of artificial neural networks whose magnetic properties would be governed with voltage.

Altres ajuts: Acord transformatiu CRUE-CSIC, Magneto-ionics allows for tunable control of magnetism by voltage-driven transport of ions, traditionally oxygen or lithium and, more recently, hydrogen, fluorine, or nitrogen. Here, magneto-ionic effects in single-layer iron nitride films are demonstrated, and their performance is evaluated at room temperature and compared with previously studied cobalt nitrides. Iron nitrides require increased activation energy and, under high bias, exhibit more modest rates of magneto-ionic motion than cobalt nitrides. Ab initio calculations reveal that, based on the atomic bonding strength, the critical field required to induce nitrogen-ion motion is higher in iron nitrides (≈6.6 V nm -1) than in cobalt nitrides (≈5.3 V nm -1). Nonetheless, under large bias (i.e., well above the magneto-ionic onset and, thus, when magneto-ionics is fully activated), iron nitride films exhibit enhanced coercivity and larger generated saturation magnetization, surpassing many of the features of cobalt nitrides. The microstructural effects responsible for these enhanced magneto-ionic effects are discussed. These results open up the potential integration of magneto-ionics in existing nitride semiconductor materials in view of advanced memory system architectures.

The utility of electrical resistivity as an indicator of magnetoionic performance in stoichiometrically and structurally similar thin-film systems is demonstrated. A series of highly nanocrystalline cobalt nitride (Co-N) thin films (85 nm thick) with a broad range of electrical properties exhibit markedly different magnetoionic behaviors. Semiconducting, near stoichiometric CoN films show the best performance, better than their metallic and insulating counterparts. Resistivity reflects the interplay between atomic bonding, carrier localization, and structural defects, and in turn determines the strength and distribution of applied electric fields inside the actuated films. This fact, generally overlooked, reveals that resistivity can be used to quickly evaluate the potential of a system to exhibit optimal magnetoionic effects, while also opening interesting challenges.

Magneto-ionics allows for tunable control of magnetism by voltage-driven transport of ions, traditionally oxygen or lithium and, more recently, hydrogen, fluorine, or nitrogen. Here, magneto-ionic effects in single-layer iron nitride films are demonstrated, and their performance is evaluated at room temperature and compared with previously studied cobalt nitrides. Iron nitrides require increased activation energy and, under high bias, exhibit more modest rates of magneto-ionic motion than cobalt nitrides. Ab initio calculations reveal that, based on the atomic bonding strength, the critical field required to induce nitrogen-ion motion is higher in iron nitrides (≈6.6 V nm-1) than in cobalt nitrides (≈5.3 V nm-1). Nonetheless, under large bias (i.e., well above the magneto-ionic onset and, thus, when magneto-ionics is fully activated), iron nitride films exhibit enhanced coercivity and larger generated saturation magnetization, surpassing many of the features of cobalt nitrides. The microstructural effects responsible for these enhanced magneto-ionic effects are discussed. These results open up the potential integration of magneto-ionics in existing nitride semiconductor materials in view of advanced memory system architectures.

Magneto-ionics, understood as voltage-driven ion transport in magnetic materials, has largely relied on controlled migration of oxygen ions. Here, we demonstrate room-temperature voltage-driven nitrogen transport (i.e., nitrogen magneto-ionics) by electrolyte-gating of a CoN film. Nitrogen magneto-ionics in CoN is compared to oxygen magneto-ionics in Co3O4. Both materials are nanocrystalline (face-centered cubic structure) and show reversible voltage-driven ON-OFF ferromagnetism. In contrast to oxygen, nitrogen transport occurs uniformly creating a plane-wave-like migration front, without assistance of diffusion channels. Remarkably, nitrogen magneto-ionics requires lower threshold voltages and exhibits enhanced rates and cyclability. This is due to the lower activation energy for ion diffusion and the lower electronegativity of nitrogen compared to oxygen. These results may open new avenues in applications such as brain-inspired computing or iontronics in general.

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 magnetically actuated devices. Boosting the induced changes in magnetization, magneto-ionic rates and cyclability continue to be key challenges to turn magneto-ionics into real applications. Here, it is demonstrated that room-temperature magneto-ionic effects in electrolyte-gated paramagnetic CoO films can be largely increased both in terms of generated magnetization (6 times larger) and speed (35 times faster) if the electric field is applied using an electrochemical capacitor configuration (utilizing an underlying conducting buffer layer) instead of placing the electric contacts at the side of the semiconductor (electric-double-layer transistor-like configuration). This is due to the greater uniformity and strength of the electric field in the capacitor design. These results are appealing to widen the use of ion migration in technological applications such as neuromorphic computing or iontronics in general.