Magnetic skyrmions are topological spin textures that can be used as information carriers for the next-generation information storage and processing. The electric-field controlling of skyrmions in such devices is essential but remains technologically challenging. Here, using the first-principles calculation and the Ginzburg-Landau theory, we propose a reliable process for writing and deleting skyrmions by electric fields, on the platform of a multiferroic heterostructure, particularly the $\text{Cr}_{2}\text{Ge}_{2}\text{Te}_{6} $/$ \text{In}_{2}\text{Se}_{3} $ heterostructure. We show that the electric field controls the electric polarization and indirectly influences the antisymmetric Dzyaloshinskii-Moriya interaction (DMI) between the magnetic moments. The latter is responsible for the generation and removal of the skyrmion spin textures, and we study this mechanism by the Ginzburg-Landau analysis. We discuss the real-space Berry curvature, topological Hall effects, possible quantum anomalous Hall effect, and other competing magnetic structures. These results represent examples of quantum technology and may have potential applications in future skyrmionics and the device fabrication.
A magnetic skyrmionium (also called 2$π$-skyrmion) can be understood as a skyrmion - a topologically non-trivial magnetic whirl - which is situated in the center of a second skyrmion with reversed magnetization. Here, we propose a new optoelectrical writing and deleting mechanism for skyrmioniums in thin films, as well as a reading mechanism based on the topological Hall voltage. Furthermore, we point out advantages for utilizing skyrmioniums as carriers of information in comparison to skyrmions with respect to the current-driven motion. We simulate all four constituents of an operating skyrmi…
This paper reports on a theoretical proposal for electrical creation of magnetic skyrmions on a thin-film specimen of a multiferroic chiral magnet by local application of an electric field, instead of an electric current, via an electrode tip. This method can be traced back to the mutual coupling between skyrmion spins and the electric polarizations in multiferroics, and represents a unique technique for use in potential skyrmion-based memory devices without Joule-heating losses.
Magnetic skyrmions, vortex-like swirling spin textures characterized by a quantized topological invariant, realized in chiral-lattice magnets are currently attracting intense research interest. In particular, their dynamics under external fields is an issue of vital importance both for fundamental science and for technical application. Whereas observations of magnetic skyrmions had been limited to metallic magnets so far, their realization was discovered also in a chiral-lattice insulating magnet Cu2OSeO3 in 2012. Skyrmions in the insulator turned out to exhibit multiferroic nature with spin-i…
Recent discovery of Skyrmion crystal phase in insulating multiferroic compound Cu$_2$OSeO$_3$ calls for new ways and ideas to manipulate the Skyrmions in the absence of spin transfer torque from the conduction electrons. It is shown here that the position-dependent electric field, pointed along the direction of the average induced dipole moment of the Skyrmion, can induce the Hall motion of Skyrmion with its velocity orthogonal to the field gradient. Finite Gilbert damping produces longitudinal motion. We find a rich variety of resonance modes excited by a.c. electric field.
We theoretically discover that unique eigenmodes of skyrmion crystal (SkX) are not only magnetically active to ac magnetic field (H^w) but also electrically active to ac electric field (E^w) in a multiferroic chiral-lattice magnet Cu2OSeO3, which amplifies the dynamical magnetoelectric coupling between E^w and the spin texture. The resulting intense interference between their electric and magnetic activation processes can lead to unprecedentedly large diode effect on the microwave, i.e., its absorption by SkX changes up to ~20% when the incident direction is reversed. Our results demonstrate t…
Broadband microwave spectroscopy has been performed on single-crystalline GaV$_4$S$_8$, which exhibits a complex magnetic phase diagram including cycloidal, Néel-type skyrmion lattice, as well as field-polarized ferromagnetic phases below 13 K. At zero and small magnetic fields two collective modes are found at 5 and 15 GHz, which are characteristic of the cycloidal state in this easy-axis magnet. In finite fields, entering the skyrmion lattice phase, the spectrum transforms into a multi-mode pattern with absorption peaks near 4, 8, and 15 GHz. The spin excitation spectra in GaV$_4$S$_8$ and t…
Cu2OSeO3 is known as a unique example of insulating multiferroic compounds with skyrmion spin texture, which is characterized by the chiral cubic crystal structure at ambient pressure. Recently, it has been reported that this compound shows pressure-induced structural transition with large enhancement of magnetic ordering temperature Tc. In the present study, we have investigated the detailed crystal structure in the high pressure phase, by combining the synchrotron X-ray diffraction experiment with the diamond anvil cell and the analysis based on the genetic algorithm. Our results suggest tha…
The lacunar spinel GaV4S8 exhibits orbital ordering at 44 K and shows a complex magnetic phase diagram below 12.7 K, which includes ferromagnetic and cycloidal spin order. At low but finite external magnetic fields, Néel-type skyrmions are formed in this material. Skyrmions are whirl-like spin vortices that have received great theoretical interest because of their non-trivial spin topology and that are also considered as basic entities for new data-storage technologies. Interestingly, we found that the orbitally ordered phase shows sizable ferroelectric polarization and that excess spin-driven…
Skyrmions are whirl like topological spin objects with high potential for future magnetic data storage. It is a fundamental question, relevant for both basic research and application, if a ferroelectric (FE) polarization can be associated with their magnetic texture and if these objects can be manipulated by electric fields. Here, we study the interplay between magnetism and electric polarization in the lacunar spinel GaV4S8, which undergoes a structural transition associated with orbital ordering at 44 K and reveals a complex magnetic phase diagram below 13 K, including a ferromagnetic (FM), …
We present a theory of magnetoelectric magnon-photon coupling in cavities hosting noncentrosymmetric magnets. Analogously to nonreciprocal phenomena in multiferroics, the magnetoelectric coupling is time-reversal and inversion asymmetric. This asymmetry establishes a means for exceptional tunability of magnon-photon coupling, which can be switched on and off by reversing the magnetization direction. Taking the multiferroic skyrmion-host Cu$_2$OSeO$_3$ with ultralow magnetic damping as an example, we reveal the electrical activity of skyrmion eigenmodes and propose it for magnon-photon splittin…
Magnetic materials in which it is possible to control the topology of their magnetic order in real space or the topology of their magnetic excitations in reciprocal space are highly sought-after as platforms for alternative data storage and computing architectures. Here we show that multiferroic insulators, owing to their magneto-electric coupling, offer a natural and advantageous way to address these two different topologies using laser fields. We demonstrate that via a delicate balance between the energy injection from a high-frequency laser and dissipation, single skyrmions -- archetypical …
We theoretically propose that magnetic skyrmion, nanometric spin vortex characterized by a quantized topological number, can be electrically created on a thin-film specimen of chiral-lattice magnetic insulator within a few nanoseconds by applying an electric field via an electrode tip taking advantage of coupling between noncollinear skyrmion spins and electric polarizations. This finding will pave a route to utilizing multiferroic skyrmions as information carriers for low-energy-consuming magnetic storage devices without Joule-heating energy losses.
GaV$_4$S$_8$ is a multiferroic semiconductor hosting magnetic cycloid (Cyc) and Néel-type skyrmion lattice (SkL) phases with a broad region of thermal and magnetic stability. Here, we use time-resolved magneto-optical Kerr spectroscopy and micro-magnetic simulations to demonstrate the coherent generation of collective spin excitations in the Cyc and SkL phases driven by an optically-induced modulation of uniaxial anisotropy. Our results shed light on spin-dynamics in anisotropic materials hosting skyrmions and pave a new pathway for the optical control of their magnetic order.
Insulating helimagnetic Cu2OSeO3 shows sizeable magnetoelectric effects in its skyrmion phase. Using magnetization measurements, magneto-current analysis and dielectric spectroscopy, we provide a thorough investigation of magnetoelectric coupling, polarization and dielectric constants of the ordered magnetic and polar phases of single-crystalline Cu2OSeO3 in external magnetic fields up to 150 mT and at temperatures below 60 K. From these measurements we construct a detailed phase diagram. Especially, the skyrmion phase and the metamagnetic transition of helical to conical spin order are charac…
We present a theoretical examination of the magneto-electric response in the recently discovered multiferroic insulator Cu$_2$OSeO$_3$. Combining Monte Carlo simulation and Ginzburg-Landau analysis we predict the response in each of the magnetic phases, including helical, conical, ferromagnetic and Skyrmion crystal phases, both for thin film and bulk systems. A common feature for all non-collinear phases is that the magneto-electric susceptibility increases linearly with the applied magnetic field. Being both calculable and measurable, the magneto-electric susceptibility can serve as a new pow…
Skyrmions are topologically protected quantum objects at the nanometre scale. They form perpendicular to an applied magnetic field at a certain temperature and arrange themselves in a typically hexagonal lattice. Using small angle neutron scattering we have determined the magnetic field versus temperature phase diagrams of the stability range of the different magnetic phases, the helical as well as the skyrmion phases in the multiferroic skyrmion material Cu$_2$OSeO$_3$. Therefore, a single crystal was mounted in different crystal orientations, i.e. unoriented and with the crystallographic $\l…
Several challenges in designing an operational Skyrmion racetrack memory are well-known. Among those challenges, a few contradictions can be identified if researchers were to rely only on metallic materials. Hence, expanding the exploration on Skyrmion Physics into oxide materials is essential to bridge the contradicting gap. In this topical review, we first briefly revise the theories and criteria involved in stabilizing and manipulating Skymions, followed by studying the behaviors of dipolar-stabilized magnetic bubbles. Next, we explore the properties of multiferroic Skyrmions with magnetoel…
Magnetic skyrmions have been the focus of intense research due to their unique qualities which result from their topological protections. Previous work on Cu$_2$OSeO$_3$, the only known insulating multiferroic skyrmion material, has shown that chemical substitution alters the skyrmion phase. We chemically substitute Zn, Ag, and S into powdered Cu$_2$OSeO$_3$ to study the effect on the magnetic phase diagram. In both the Ag and the S substitutions, we find that the skyrmion phase is stabilized over a larger temperature range, as determined via magnetometry and small-angle neutron scattering (SA…
The lack of inversion symmetry in the crystal lattice of magnetic materials gives rise to complex non-collinear spin orders through interactions of relativistic nature, resulting in interesting physical phenomena, such as emergent electromagnetism. Studies of cubic chiral magnets revealed a universal magnetic phase diagram, composed of helical spiral, conical spiral and skyrmion crystal phases. Here, we report a remarkable deviation from this universal behavior. By combining neutron diffraction with magnetization measurements we observe a new multi-domain state in Cu2OSeO3. Just below the uppe…
We report on the anomalous magnetization dynamics of the cycloidally-modulated spin textures under the influence of uniaxial anisotropy in multiferroic $\mathrm{GaV_4S_8}$. The temperature and field dependence of the linear ac susceptibility [$χ_{1ω}^{\prime}(T,H)$], ac magnetic loss [$χ_{1ω}^{\prime\prime}(T,H)$], and nonlinear ac magnetic response [$M_{3ω}(T,H)$] are examined across the magnetic phase diagram in the frequency range $f = 10-10000$ Hz. According to recent theory, skyrmion vortices under axial crystal symmetry are confined along specific orientations, resulting in enhanced robu…
This article presents a survey of many nontrivial effects connected with the coupling of electric and magnetic degrees of freedom in solids -- the field initiated by I.~E.~Dzyaloshinskii in 1959. I briefly consider the main physics of ultiferroic materials, and concentrate on different effects "beyond multiferroics", based on the same physical mechanisms which operate in multiferroics. In particular they lead to nontrivial electric properties of different magnetic textures -- such as the appearance of dipoles on magnetic monopoles in spin ice, dipoles on some domain walls in the usual ferromag…
We report on the slow magnetization dynamics observed upon the magnetic phase transitions of GaV4S8, a multiferroic compound featuring a long-ranged cycloidal magnetic order and a Néel-type skyrmion lattice in a relatively broad temperature range below its Curie temperature. The fundamental difference between GaV4S8 and the chiral helimagnets, wherein the skyrmion phase was first discovered, lies within the polar symmetry of GaV4S8, promoting a cycloidal instead of a helical magnetic order and rendering the magnetic phase diagram essentially different from that in the cubic helimagnets. Our ac…
Using SQUID magnetometry techniques, we have studied the change in magnetization versus applied ac electric field, i.e. the magnetoelectric (ME) susceptibility dM/dE, in the chiral-lattice ME insulator Cu2OSeO3. Measurements of the dM/dE response provide a sensitive and efficient probe of the magnetic phase diagram, and we observe clearly distinct responses for the different magnetic phases, including the skyrmion lattice phase. By combining our results with theoretical calculation, we estimate quantitatively the ME coupling strength as λ = 0.0146 meV/(V/nm) in the conical phase. Our study dem…
Small angle neutron scattering experiments were performed on a bulk single crystal of chiral-lattice multiferroic insulator Cu$_2$OSeO$_3$. In the absence of an external magnetic field, helical spin order with magnetic modulation vector $q \parallel <001>$ was identified. When a magnetic field is applied, a triple-$q$ magnetic structure emerges normal to the field in the A-phase just below the magnetic ordering temperature $T_c$, which suggests the formation of a triangular lattice of skyrmions. Notably, the favorable $q$-direction in the A-phase changes from $q \parallel <110>$ to $q \paralle…
The lacunar spinel GaV$_{4}$S$_{8}$ was recently suggested to be a prototype multiferroic material hosting skyrmion lattice states with a sizeable polarization $\boldsymbol{P}$ coupled to magnetic order. We explain this phenomenon on the microscopic level. On the basis of density functional theory, we construct an effective model describing the behavior of magnetically active electrons in a weakly coupled lattice formed by molecular orbitals of the (V$_{4}$S$_{4}$)$^{5+}$ clusters. By applying superexchange theory combined with the Berry-phase theory for $\boldsymbol{P}$, we derive a compass m…
We have carried out neutron diffraction and small angle neutron scattering measurements on a high quality single crystal of the cubic lacunar spinel multiferroic, GaV$_4$S$_8$, as a function of magnetic field and temperature to determine the magnetic properties for the single electron that is located on the tetrahedrally coordinated V$_4$ molecular unit. Our results are in good agreement with the structural transition at 44 K from cubic to rhombohedral symmetry where the system becomes a robust ferroelectric, while long range magnetic order develops below 13 K in the form of an incommensurate …
Complex low-temperature ordered states in chiral magnets are typically governed by a competition between multiple magnetic interactions. The chiral-lattice multiferroic Cu2OSeO3 became the first insulating helimagnetic material in which a long-range order of topologically stable spin vortices known as skyrmions was established. Here we employ state-of-the-art inelastic neutron scattering (INS) to comprehend the full three-dimensional spin excitation spectrum of Cu2OSeO3 over a broad range of energies. Distinct types of high- and low-energy dispersive magnon modes separated by an extensive ener…
Electric field control of magnetic structures, particularly topological defects in magnetoelectric materials, draws a great attention in recent years, which has led to experimental success in creation and manipulation by electric field of single magnetic defects, such as domain walls and skyrmions. In this work we explore a scenario of electric field creation of another type of topological defects -- magnetic vortices and antivortices, which are characteristic for materials with easy plane (XY) symmetry. Each magnetic (anti)vortex in magnetoelectric materials (such as type-II multiferroics) po…
