Electron holography observation of individual ferrimagnetic lattice planes.

Atomic-scale observations of a specific local area would be considerably beneficial when exploring new fundamental materials and devices. The development of hardware-type aberration correction1,2 in electron microscopy has enabled local structural observations with atomic resolution3-5 as well as chemical and vibration analysis6-8. In magnetic imaging, however, atomic-level spin configurations are analysed by electron energy-loss spectroscopy by placing samples in strong magnetic fields9-11, which destroy the nature of the magnetic ordering in the samples. Although magnetic-field-free observations can visualize the intrinsic magnetic fields of an antiferromagnet by unit-cell averaging12, directly observing the magnetic field of an individual atomic layer of a non-uniform structure is challenging. Here we report that the magnetic fields of an individual lattice plane inside materials with a non-uniform structure can be observed under magnetic-field-free conditions by electron holography with a hardware-type aberration corrector assisted by post-digital aberration correction. The magnetic phases of the net magnetic moments of (111) lattice planes formed by opposite spin orderings between Fe3+ and Mo5+ in a ferrimagnetic double-perovskite oxide (Ba2FeMoO6) were successfully observed. This result opens the door to direct observations of the magnetic lattice in local areas, such as interfaces and grain boundaries, in many materials and devices.

Large nonlinear optical magnetoelectric response in a noncentrosymmetric magnetic Weyl semimetal.

Weyl semimetals resulting from either inversion (P) or time-reversal (T) symmetry breaking have been revealed to show the record-breaking large optical response due to intense Berry curvature of Weyl-node pairs. Different classes of Weyl semimetals with both P and T symmetry breaking potentially exhibit optical magnetoelectric (ME) responses, which are essentially distinct from the previously observed optical responses in conventional Weyl semimetals, leading to the versatile functions such as directional dependence for light propagation and gyrotropic effects. However, such optical ME phenomena of (semi)metallic systems have remained elusive so far. Here, we show the large nonlinear optical ME response in noncentrosymmetric magnetic Weyl semimetal PrAlGe, in which the polar structural asymmetry and ferromagnetic ordering break P and T symmetry. We observe the giant second harmonic generation (SHG) arising from the P symmetry breaking in the paramagnetic phase, being comparable to the largest SHG response reported in Weyl semimetal TaAs. In the ferromagnetically ordered phase, it is found that interference between this nonmagnetic SHG and the magnetically induced SHG emerging due to both P and T symmetry breaking results in the magnetic field switching of SHG intensity. Furthermore, such an interference effect critically depends on the light-propagating direction. The corresponding magnetically induced nonlinear susceptibility is significantly larger than the prototypical ME material, manifesting the existence of the strong nonlinear dynamical ME coupling. The present findings establish the unique optical functionality of P- and T-symmetry broken ME topological semimetals.

Emergent electromagnetic induction in a helical-spin magnet.

An inductor, one of the most fundamental circuit elements in modern electronic devices, generates a voltage proportional to the time derivative of the input current1. Conventional inductors typically consist of a helical coil and induce a voltage as a counteraction to time-varying magnetic flux penetrating the coil, following Faraday's law of electromagnetic induction. The magnitude of this conventional inductance is proportional to the volume of the inductor's coil, which hinders the miniaturization of inductors2. Here, we demonstrate an inductance of quantum-mechanical origin3, generated by the emergent electric field induced by current-driven dynamics of spin helices in a magnet. In microscale rectangular magnetic devices with nanoscale spin helices, we observe a typical inductance as large as -400 nanohenry, comparable in magnitude to that of a commercial inductor, but in a volume about a million times smaller. The observed inductance is enhanced by nonlinearity in current and shows non-monotonous frequency dependence, both of which result from the current-driven dynamics of the spin-helix structures. The magnitude of the inductance rapidly increases with decreasing device cross-section, in contrast to conventional inductors. Our findings may pave the way to microscale, simple-shaped inductors based on emergent electromagnetism related to the quantum-mechanical Berry phase.

Task-adaptive physical reservoir computing.

Reservoir computing is a neuromorphic architecture that may offer viable solutions to the growing energy costs of machine learning. In software-based machine learning, computing performance can be readily reconfigured to suit different computational tasks by tuning hyperparameters. This critical functionality is missing in 'physical' reservoir computing schemes that exploit nonlinear and history-dependent responses of physical systems for data processing. Here we overcome this issue with a 'task-adaptive' approach to physical reservoir computing. By leveraging a thermodynamical phase space to reconfigure key reservoir properties, we optimize computational performance across a diverse task set. We use the spin-wave spectra of the chiral magnet Cu2OSeO3 that hosts skyrmion, conical and helical magnetic phases, providing on-demand access to different computational reservoir responses. The task-adaptive approach is applicable to a wide variety of physical systems, which we show in other chiral magnets via above (and near) room-temperature demonstrations in Co8.5Zn8.5Mn3 (and FeGe).

A correlated ferromagnetic polar metal by design.

Polar metals have recently garnered increasing interest because of their promising functionalities. Here we report the experimental realization of an intrinsic coexisting ferromagnetism, polar distortion and metallicity in quasi-two-dimensional Ca3Co3O8. This material crystallizes with alternating stacking of oxygen tetrahedral CoO4 monolayers and octahedral CoO6 bilayers. The ferromagnetic metallic state is confined within the quasi-two-dimensional CoO6 layers, and the broken inversion symmetry arises simultaneously from the Co displacements. The breaking of both spatial-inversion and time-reversal symmetries, along with their strong coupling, gives rise to an intrinsic magnetochiral anisotropy with exotic magnetic field-free non-reciprocal electrical resistivity. An extraordinarily robust topological Hall effect persists over a broad temperature-magnetic field phase space, arising from dipole-induced Rashba spin-orbit coupling. Our work not only provides a rich platform to explore the coupling between polarity and magnetism in a metallic system, with extensive potential applications, but also defines a novel design strategy to access exotic correlated electronic states.

Real-space determination of the isolated magnetic skyrmion deformation under electric current flow.

The manipulation and control of electron spins, the fundamental building blocks of magnetic domains and spin textures, are at the core of spintronics. Of particular interest is the effect of the electric current on topological magnetic skyrmions, such as the current-induced deformation of isolated skyrmions. The deformation has consequences ranging from perturbed dynamics to modified packing configurations. In this study, we measured the current-driven real-space deformation of isolated, pinned skyrmions within Co10Zn10 at room temperature. We observed that the skyrmions are surprisingly soft, readily deforming during electric current application into an elliptical shape with a well-defined deformation axis (semimajor axis). We found that this axis rotates unidirectionally toward the current direction irrespective of electric current polarity and that the elliptical deformation reverses back upon current termination. We quantified the average distortion δ, which increased by ∼90% during the largest applied current density |j| = 8.46 ×109 A/m2 when compared with the skyrmion's intrinsic shape ([Formula: see text]). Additionally, we demonstrated an approximately 120% average skyrmion core size expansion during current application, highlighting the skyrmions' inherent topological protection. This evaluation of in situ electric current-induced skyrmion deformation paints a clearer picture of spin-polarized electron-skyrmion interactions and may prove essential in designing spintronic devices.

Photovoltaic effect by soft phonon excitation.

SignificanceThe quantum-mechanical geometric phase of electrons provides various phenomena such as the dissipationless photocurrent generation through the shift current mechanism. So far, the photocurrent generations are limited to above or near the band-gap photon energy, which contradicts the increasing demand of the low-energy photonic functionality. We demonstrate the photocurrent through the optical phonon excitations in ferroelectric BaTiO3 by using the terahertz light with photon energy far below the band gap. This photocurrent without electron-hole pair generation is never explained by the semiclassical treatment of electrons and only arises from the quantum-mechanical geometric phase. The observed photon-to-current conversion efficiency is as large as that for electronic excitation, which can be well accounted for by newly developed theoretical formulation of shift current.

Emergent electromagnetic induction beyond room temperature.

Emergent electromagnetic induction based on electrodynamics of noncollinear spin states may enable dramatic miniaturization of inductor elements widely used in electric circuits, yet the research is still in its infancy and many issues must be resolved toward its application. One such problem is how to increase working temperature to room temperature, and possible thermal agitation effects on the quantum process of the emergent induction are unknown. We report here large emergent electromagnetic induction achieved around and above room temperature, making use of a few tens of micrometer-sized devices based on the high-temperature (up to 330 K) and short-period (≤ 3 nm) spin-spiral states of a metallic helimagnet. The observed inductance value L and its sign are observed to vary to a large extent, depending not only on the spin-helix structure controlled by temperature and applied magnetic field but also on the applied current density. The present finding on room-temperature operation and possible sign control of L may provide a step toward realizing microscale quantum inductors on the basis of emergent electromagnetism in spin-helix states.

Large Hall and Nernst responses from thermally induced spin chirality in a spin-trimer ferromagnet.

The long-range order of noncoplanar magnetic textures with scalar spin chirality (SSC) can couple to conduction electrons to produce an additional (termed geometrical or topological) Hall effect. One such example is the Hall effect in the skyrmion lattice state with quantized SSC. An alternative route to attain a finite SSC is via the spin canting caused by thermal fluctuations in the vicinity of the ferromagnetic ordering transition. Here, we report that for a highly conducting ferromagnet with a two-dimensional array of spin trimers, the thermally generated SSC can give rise to a gigantic geometrical Hall conductivity even larger than the intrinsic anomalous Hall conductivity of the ground state. We also demonstrate that the SSC induced by thermal fluctuations leads to a strong response in the Nernst effect. A comparison of the sign and magnitude of fluctuation-Nernst and Hall responses in fundamental units indicates the need for a momentum-space picture to model these thermally induced signals.

Berry curvature generation detected by Nernst responses in ferroelectric Weyl semimetal.

The quest for nonmagnetic Weyl semimetals with high tunability of phase has remained a demanding challenge. As the symmetry-breaking control parameter, the ferroelectric order can be steered to turn on/off the Weyl semimetals phase, adjust the band structures around the Fermi level, and enlarge/shrink the momentum separation of Weyl nodes which generate the Berry curvature as the emergent magnetic field. Here, we report the realization of a ferroelectric nonmagnetic Weyl semimetal based on indium-doped Pb1- x Sn x Te alloy in which the underlying inversion symmetry as well as mirror symmetry are broken with the strength of ferroelectricity adjustable via tuning the indium doping level and Sn/Pb ratio. The transverse thermoelectric effect (i.e., Nernst effect), both for out-of-plane and in-plane magnetic field geometry, is exploited as a Berry curvature-sensitive experimental probe to manifest the generation of Berry curvature via the redistribution of Weyl nodes under magnetic fields. The results demonstrate a clean, nonmagnetic Weyl semimetal coupled with highly tunable ferroelectric order, providing an ideal platform for manipulating the Weyl fermions in nonmagnetic systems.

Topological spintronics and magnetoelectronics.

Topological electronic materials, such as topological insulators, are distinct from trivial materials in the topology of their electronic band structures that lead to robust, unconventional topological states, which could bring revolutionary developments in electronics. This Perspective summarizes developments of topological insulators in various electronic applications including spintronics and magnetoelectronics. We group and analyse several important phenomena in spintronics using topological insulators, including spin-orbit torque, the magnetic proximity effect, interplay between antiferromagnetism and topology, and the formation of topological spin textures. We also outline recent developments in magnetoelectronics such as the axion insulator and the topological magnetoelectric effect observed using different topological insulators.

Geometrically stabilized skyrmionic vortex in FeGe tetrahedral nanoparticles.

The concept of topology has dramatically expanded the research landscape of magnetism, leading to the discovery of numerous magnetic textures with intriguing topological properties. A magnetic skyrmion is an emergent topological magnetic texture with a string-like structure in three dimensions and a disk-like structure in one and two dimensions. Skyrmions in zero dimensions have remained elusive due to challenges from many competing orders. Here, by combining electron holography and micromagnetic simulations, we uncover the real-space magnetic configurations of a skyrmionic vortex structure confined in a B20-type FeGe tetrahedral nanoparticle. An isolated skyrmionic vortex forms at the ground state and this texture shows excellent robustness against temperature without applying a magnetic field. Our findings shed light on zero-dimensional geometrical confinement as a route to engineer and manipulate individual skyrmionic metastructures.

Spin-Lattice and Magnetoelectric Couplings Enhanced by Orbital Degrees of Freedom in Polar Multiferroic Semiconductors.

Orbital degrees of freedom mediating an interaction between spin and lattice were predicted to raise strong magnetoelectric effect, i.e., to realize an efficient coupling between magnetic and ferroelectric orders. However, the effect of orbital fluctuations has been considered only in a few magnetoelectric materials, as orbital-degeneracy driven Jahn-Teller effect rarely couples to polarization. Here, we explore the spin-lattice coupling in multiferroic Swedenborgites with mixed valence and Jahn-Teller active transition metal ions on a stacked triangular and Kagome lattice using infrared and dielectric spectroscopy. On one hand, in CaBaM_{4}O_{7} (M=Co, Fe), we observe a strong magnetic-order-induced shift in the phonon frequencies and a corresponding large change in the dielectric response. Remarkably, as an unusual manifestation of the spin-phonon coupling, the spin fluctuations reduce the phonon lifetime by one order of magnitude at the magnetic phase transitions. On the other hand, lattice vibrations, dielectric response, and electric polarization show no variation at the Néel temperature of CaBaFe_{2}Co_{2}O_{7}, which is built up by orbital singlet ions. Our results provide a showcase for orbital degrees of freedom enhanced magnetoelectric coupling via the example of Swedenborgites.

Kagome Lattice Promotes Chiral Spin Fluctuations.

Dynamical spin fluctuations in magnets can be endowed with a slight bent toward left- or right-handed chirality by Dzyaloshinskii-Moriya interactions. However, little is known about the crucial role of lattice geometry on these chiral spin fluctuations and on fluctuation-related transport anomalies driven by the quantum-mechanical (Berry) phase of conduction electrons. Via thermoelectric Nernst effect and electric Hall effect experiments, we detect chiral spin fluctuations in the paramagnetic regime of a kagome lattice magnet; these signals are largely absent in a comparable triangular lattice magnet. Supported by Monte Carlo calculations, we identify lattices with at least two dissimilar plaquettes as most promising for Berry phase phenomena driven by thermal fluctuations in paramagnets.

Magnetic Skyrmion Materials.

Skyrmion, a concept originally proposed in particle physics half a century ago, can now find the most fertile field for its applicability, that is, the magnetic skyrmion realized in helimagnetic materials. The spin swirling vortex-like texture of the magnetic skyrmion can define the particle nature by topology; that is, all the constituent spin moments within the two-dimensional sheet wrap the sphere just one time. Such a topological nature of the magnetic skyrmion can lead to extraordinary metastability via topological protection and the driven motion with low electric-current excitation, which may promise future application to spintronics. The skyrmions in the magnetic materials frequently show up as the crystal lattice form, e.g., hexagonal lattice, but sometimes as isolated or independent particles. These skyrmions in magnets were initially found in acentric magnets, such as chiral, polar, and bilayered magnets endowed with antisymmetric spin exchange interaction, while the skyrmion host materials have been explored in a broader family of compounds including centrosymmetric magnets. This review describes the materials science and materials chemistry of magnetic skyrmions using the classification scheme of the skyrmion forming microscopic mechanisms. The emergent phenomena and functions mediated by skyrmions are described, including the generation of emergent magnetic and electric field by statics and dynamics of skrymions and the inherent magnetoelectric effect. The other important magnetic topological defects in two or three dimensions, such as biskyrmions, antiskyrmions, merons, and hedgehogs, are also reviewed in light of their interplay with the skyrmions.

Electric-field control of tri-state phase transformation with a selective dual-ion switch.

Materials can be transformed from one crystalline phase to another by using an electric field to control ion transfer, in a process that can be harnessed in applications such as batteries, smart windows and fuel cells. Increasing the number of transferrable ion species and of accessible crystalline phases could in principle greatly enrich material functionality. However, studies have so far focused mainly on the evolution and control of single ionic species (for example, oxygen, hydrogen or lithium ions). Here we describe the reversible and non-volatile electric-field control of dual-ion (oxygen and hydrogen) phase transformations, with associated electrochromic and magnetoelectric effects. We show that controlling the insertion and extraction of oxygen and hydrogen ions independently of each other can direct reversible phase transformations among three different material phases: the perovskite SrCoO3-δ (ref. 12), the brownmillerite SrCoO2.5 (ref. 13), and a hitherto-unexplored phase, HSrCoO2.5. By analysing the distinct optical absorption properties of these phases, we demonstrate selective manipulation of spectral transparency in the visible-light and infrared regions, revealing a dual-band electrochromic effect that could see application in smart windows. Moreover, the starkly different magnetic and electric properties of the three phases-HSrCoO2.5 is a weakly ferromagnetic insulator, SrCoO3-δ is a ferromagnetic metal, and SrCoO2.5 is an antiferromagnetic insulator-enable an unusual form of magnetoelectric coupling, allowing electric-field control of three different magnetic ground states. These findings open up opportunities for the electric-field control of multistate phase transformations with rich functionalities.

Defect tolerant zero-bias topological photocurrent in a ferroelectric semiconductor.

Lattice defect is a major cause of energy dissipation in conventional electric current due to the drift and diffusion motions of electrons. Different nature of current emerges when noncentrosymmetric materials are excited by light. This current, called the shift current, originates from the change in the Berry connection of electrons' wave functions during the interband optical transition. Here, we demonstrate the defect tolerance of shift current using single crystals of ferroelectric semiconductor antimony sulfoiodide (SbSI). Although the dark conductance spreads over several orders of magnitude in each crystal due to the difference in the density of defect levels, the observed shift current converges to an identical value. We also reveal that the shift current is scarcely disturbed by the surface defects while they drastically suppress the conventional photocurrent. The defect tolerance is a manifestation of the topological nature of shift current, which will be a crucial advantage in optoelectronic applications.

Real-Space Observations of Three-Dimensional Antiskyrmions and Skyrmion Strings.

Nanometric topological spin textures, such as skyrmions (Sks) and antiskyrmions (antiSks), have attracted much attention recently. However, most studies have focused on two-dimensional spin textures in films with inherent or synthetic antisymmetric spin-exchange interaction, termed Dzyaloshinskii-Moriya interaction, although three-dimensional (3D) topological spin textures, such as antiSks composed of alternating Bloch- and Néel-type spin spirals, chiral bobbers carrying emergent magnetic monopoles, and deformed Sk strings, are ubiquitous. To elucidate these textures, we have developed a 3D nanometric magnetic imaging technique, tomographic Lorentz transmission electron microscopy (TEM). The approach enables the visualization of the 3D shape of magnetic objects and their 3D vector field mapping. Here we report 3D vector field maps of deformed Sk-strings and antiSk using the technique. This research approach will lead to discoveries and understanding of fertile 3D magnetic structures in a broad class of magnets, providing insight into 3D topological magnetism.

Detection of Topological Spin Textures via Nonlinear Magnetic Responses.

Topologically nontrivial spin textures, such as skyrmions and dislocations, display emergent electrodynamics and can be moved by spin currents over macroscopic distances. These unique properties and their nanoscale size make them excellent candidates for the development of next-generation race-track memory and unconventional computing. A major challenge for these applications and the investigation of nanoscale magnetic structures in general is the realization of suitable detection schemes. We study magnetic disclinations, dislocations, and domain walls in FeGe and reveal pronounced responses that distinguish them from the helimagnetic background. A combination of magnetic force microscopy (MFM) and micromagnetic simulations links the response to the local magnetic susceptibility, that is, characteristic changes in the spin texture driven by the MFM tip. On the basis of the findings, which we explain using nonlinear response theory, we propose a read-out scheme using superconducting microcoils, presenting an innovative approach for detecting topological spin textures and domain walls in device-relevant geometries.

Entropy-Assisted, Long-Period Stacking of Honeycomb Layers in an AlB2-Type Silicide.

Configurational entropy can impact crystallization processes, tipping the scales between structures of nearly equal internal energy. Using alloyed single crystals of Gd2PdSi3 in the AlB2-type structure, we explore the formation of complex layer sequences made from alternating, two-dimensional triangular and honeycomb slabs. A four-period and an eight-period stacking sequence are found to be very close in internal energy, the latter being favored by entropy associated with covering the full configuration space of interlayer bonds. Possible consequences of polytype formation on magnetism in Gd2PdSi3 are discussed.