Néel-type Skyrmion Lattice with Confined Orientation in the Polar Magnetic Semiconductor GaV$_4$S$_8$
I. Kézsmárki, S. Bordács, P. Milde, E. Neuber, L. M. Eng, J. S. White, H. M. Rønnow, C. D. Dewhurst, M. Mochizuki, K. Yanai, H. Nakamura, D. Ehlers, V. Tsurkan, A. Loidl
继早期预测的Skyrmion晶格（SkL）-自旋涡旋的周期性阵列-最近已在各种磁性晶体中观察到，主要是手性结构。尽管具有C $_{nv}$对称性的非手性但极性晶体在开创性的理论研究中被确定为理想的SkL宿主，但SkL的原型仍然未被实验探索。在这里，我们报告的发现SkL的极性磁性半导体GaV $_4$ S $_8$菱形（C $_{3v}$）对称性和易轴各向异性。与其他大块晶体相比，SkL存在于异常宽的温度范围内，并且涡旋的取向不受外部磁场的控制，而是与磁易轴相一致。支持理论将这些独特的特征归因于一种新的非手性或Néel型SkL，它可以描述为自旋摆线的叠加，而手性磁体中的布洛赫型SkL则可以描述为自旋螺旋。
英文摘要：
Following the early prediction of the skyrmion lattice (SkL) - a periodic array of spin vortices - it has been observed recently in various magnetic crystals mostly with chiral structure. Although non-chiral but polar crystals with C$_{nv}$ symmetry were identifed as ideal SkL hosts in pioneering theoretical studies this archetype of SkL has remained experimentally unexplored. Here, we report the discovery of a SkL in the polar magnetic semiconductor GaV$_4$S$_8$ with rhombohedral (C$_{3v}$) symmetry and easy axis anisotropy. The SkL exists over an unusually broad temperature range compared with other bulk crystals and the orientation of the vortices is not controlled by the external magnetic feld but instead confned to the magnetic easy axis. Supporting theory attributes these unique features to a new non-chiral or Néel-type of SkL describable as a superposition of spin cycloids in contrast to the Bloch-type SkL in chiral magnets described in terms of spin helices.
We report the feasibility of using magnetoentropic mapping for the rapid identification of magnetic cycloid and skyrmion phases in uniaxial systems, based on the GaV4S8 and GaV4Se8 model skyrmion hosts with easy-axis and easy-plane anisotropies respectively. We show that these measurements can be interpreted with the help of a simple numerical model for the spin Hamiltonian to yield unambiguous assignments for both single phase regions and phase boundaries. In the two lacunar spinel chemistries, we obtain excellent agreement between the measured magnetoentropic features and a minimal spin Hami…
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.
The orientation of Néel-type skyrmions in the lacunar spinels GaV$_4$S$_8$ and GaV$_4$Se$_8$ is tied to the polar axes of their underlying crystal structure through the Dzyaloshinskii-Moriya interaction. In these crystals, the skyrmion lattice phase exists for externally applied magnetic fields parallel to these axes and withstands oblique magnetic fields up to some critical angle. Here, we map out the stability of the skyrmion lattice phase in both crystals as a function of field angle and magnitude using dynamic cantilever magnetometry. The measured phase diagrams reproduce the major feature…
We present the results of a muon-spin spectroscopy investigation of GaV$_4$S$_{8-y}$Se$_{y}$ with $y=0, 2, 4$ and 8. Zero-field measurements suggest that GaV$_{4}$Se$_{8}$ and GaV$_{4}$S$_{8}$ have distinct magnetic ground states, with the latter material showing an anomalous temperature-dependence of the local magnetic field. It is not possible to evolve the magnetic state continuously between these two systems, with the intermediate $y=2$ and $4$ materials showing glassy magnetic behaviour at low temperature. The skyrmion lattice (SkL) phase is evident in the $y=0$ and 8 materials through an…
Polycrystalline members of the GaV$_4$S$_{8-y}$Se$_y$ family of materials with small levels of substitution between $0 \leq y \leq 0.5$ and $7.5 \leq y\leq 8$ have been synthesized in order to investigate their magnetic and structural properties. Substitutions to the skyrmion hosting parent compounds GaV$_4$S$_8$ and GaV$_4$Se$_8$, are found to suppress the temperature of the cubic to rhombohedral structural phase transition that occurs in both end compounds and to create a temperature region around the transition where there is a coexistence of these two phases. Similarly, the magnitude of th…
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…
The GaV$_4$S$_{8-y}$Se$_y$ $(y = 0$ to $8)$ family of materials have been synthesized in both polycrystalline and single crystal form, and their structural and magnetic properties thoroughly investigated. Each of these materials crystallizes in the $F\bar{4}3m$ space group at ambient temperature. However, in contrast to the end members GaV$_4$S$_8$ and GaV$_4$Se$_8$, that undergo a structural transition to the $R3m$ space group at 42 and 41 K respectively, the solid solutions $(y = 1$ to $7)$ retain cubic symmetry down to 1.5 K. In zero applied field the end members of the family order ferroma…
GaV$_4$S$_8$ is a multiferroic semiconductor hosting N{é}el-type magnetic skyrmions dressed with electric polarization. At T$_s$ = 42K, the compound undergoes a structural phase transition of weakly first-order, from a non-centrosymmetric cubic phase at high temperatures to a polar rhombohedral structure at low temperatures. Below T$_s$, ferroelectric domains are formed with the electric polarization pointing along any of the four $\left< 111 \right>$ axes. Although in this material the size and the shape of the ferroelectric-ferroelastic domains may act as important limiting factors in the fo…
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…
Polar lacunar spinels, such as GaV$_4$S$_8$ and GaV$_4$Se$_8$, were proposed to host skyrmion phases under magnetic field. In this work, we put forward, as a candidate for Néel-type skyrmion lattice, the isostructural GaMo$_4$S$_8$, here systematically studied via both first-principles calculations and Monte Carlo simulations of model Hamiltonian. Electric polarization, driven by Jahn-Teller distortion, is predicted to arise in GaMo$_4$S$_8$, showing a comparable size but an opposite sign with respect to that evaluated in V-based counterparts and explained in terms of different electron counti…
The magnetic ground state of polycrystalline Néel skyrmion hosting material GaV$_4$S$_8$ has been investigated using ac susceptibility and powder neutron diffraction. In the absence of an applied magnetic field GaV$_4$S$_8$ undergoes a transition from a paramagnetic to a cycloidal state below 13~K and then to a ferromagnetic-like state below 6~K. With evidence from ac susceptibility and powder neutron diffraction, we have identified the commensurate magnetic structure at 1.5 K, with ordered magnetic moments of $0.23(2)~μ_{\mathrm{B}}$ on the V1 sites and $0.22(1)~μ_{\mathrm{B}}$ on the V2 site…
Magnetic skyrmions are promising candidates for future information technology. Here, we present a micromagnetic study of isolated skyrmions and skyrmion clusters in ferromagnetic nanodisks driven by the spin-polarized current with spatially varied polarization. The current-driven skyrmion clusters can be either dynamic steady or static, depending on the spatially varied polarization profile. For the dynamic steady state, the skyrmion cluster moves in a circle in the nanodisk, while for the static state, the skyrmion cluster is static. The frequency of the circular motion of skyrmion is also st…
We predict the occurrence of metastable skyrmionic spin structures such as antiskyrmions and higher-order skyrmions in ultra-thin transition-metal films at surfaces using Monte Carlo simulations based on a spin Hamiltonian parametrized from density functional theory calculations. We show that such spin structures will appear with a similar contrast in spin-polarized scanning tunneling microscopy (SP-STM) images. Both skyrmions and antiskyrmions display a circular shape for out-of-plane magnetized tips and a two-lobe butterfly contrast for in-plane tips. An unambiguous distinction can be achiev…
Topological phases such as polar skyrmions have been a fertile playground for ferroelectric oxide superlattices, with exotic physical phenomena such as negative capacitance. Herein, using phase-field simulations, we demonstrate the local control of the skyrmion phase with electric potential applied through a top electrode. Under a relatively small electric potential, the skyrmions underneath the electrode can be erased and recovered reversibly. A topologically protected transition from the symmetric to asymmetric skyrmion bubbles is observed at the edge of the electrode. While a topological tr…
We study a two-dimensional electron gas exchanged-coupled to a system of classical magnetic ions. For large Rashba spin-orbit coupling a single electron can become self-trapped in a skyrmion spin texture self-induced in the magnetic ions system. This new quasiparticle carries electrical and topological charge as well as a large spin, and we named it as magnetic skyrmionic polaron. We study the range of parameters; temperature, exchange coupling, Rashba coupling and magnetic field, for which the magnetic skyrmionic polaron is the fundamental state in the system. The dynamics of this quasipartic…
From picometre displacements to a three-dimensional lattice gas of polar skyrmions
ETH Zürich（苏黎世联邦理工学院）；Argonne National Laboratory（阿贡国家实验室）；Institute of physics, Zagreb（萨格勒布物理研究所）；Luxembourg Institute of Science and Technology（卢森堡科学与技术研究院）；Aarhus University（奥胡斯大学）
Magnetic skyrmions are particle-like topological excitations in ferromagnets, which have the topological number $Q=\pm 1$, and hence show the skyrmion Hall effect (SkHE) due to the Magnus force effect originating from the topology. Here, we propose the counterpart of the magnetic skyrmion in the antiferromagnetic (AFM) system, that is, the AFM skyrmion, which is topologically protected but without showing the SkHE. Two approaches for creating the AFM skyrmion have been described based on micromagnetic lattice simulations: (i) by injecting a vertical spin-polarized current to a nanodisk with th…
Thermally Configurable Multi-Order Polar Skyrmions in Multiferroic Oxide Superlattices
State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University（浙江大学材料科学与工程学院硅与先进半导体材料省部共建国家重点实验室）；Zhejiang Key Laboratory of Advanced Solid State Energy Storage Technology and Applications, Taizhou Institute of Zhejiang University（浙江工业大学储能技术与应用浙江省重点实验室台州研究院）；Institute of Fundamental and Transdisciplinary Research, Zhejiang University（浙江大学基础与交叉科学研究院）；School of Engineering, Hangzhou City University（杭州城市学院工学院）；College of Materials Science and Engineering, Zhejiang University of Technology（浙江工业大学材料科学与工程学院）
Room-temperature polar skyrmion bubbles that are recently found in oxide superlattice, have received enormous interests for their potential applications in nanoelectronics due to the nanometer size, emergent chirality, and negative capacitance. For practical applications, the ability to controllably manipulate them by using external stimuli is prerequisite. Here, we study the dynamics of individual polar skyrmion bubbles at the nanoscale by using in situ biasing in a scanning transmission electron microscope. The reversible electric field-driven phase transition between topological and trivial…
Polar bubble domains are complex topological defects akin to magnetic skyrmions that can spontaneously form in ferroelectric thin films and superlattices. They can be deterministically written and deleted and exhibit a set of properties, such as sub-10 nm radius and room-temperature stability, that are highly attractive for dense data storage and reconfigurable nano-electronics technologies. However, possibilities of controlled motion of electric bubble skyrmions, a critical technology requirement currently remains missing. Here we present atomistic simulations that demonstrate how external el…
The controllable phase transition and nanopatterning of topological states in a ferroelectric system under external stimuli are critical for realizing the potential applications in nanoelectronic devices such as logic, memory, race-track, etc. Herein, using the phase-field simulations, we demonstrate the mechanical manipulation of polar skyrmions in ferroelectric superlattices by applying external local compressive stress through an atomic force microscopy (AFM) tip. Different switching pathways are observed: under small to moderate force (<1 uN), the skyrmions coalesce to form a long stripe; …
Polar skyrmions are predicted to emerge from the interplay of elastic, electrostatic and gradient energies, in contrast to the key role of the anti-symmetric Dzyalozhinskii-Moriya interaction in magnetic skyrmions. With the discovery of topologically-stable polar skyrmions, it is of both fundamental and practical interest to understand the microscopic nature and the possibility of temperature- and strain-driven phase transitions in ensembles of such polar skyrmions. Here, we explore the reversible transition from a skyrmion state (topological charge of -1) to a two-dimensional, tetratic lattic…
Skyrmions are topological magnetic textures that can arise in non-centrosymmetric ferromagnetic materials. In most systems experimentally investigated to date, skyrmions emerge as classical objects. However, the discovery of skyrmions with nanometer length scales has sparked interest in their quantum properties. Here, we simulate the ground states of two-dimensional spin-$1/2$ Heisenberg lattices with Dzyaloshinskii-Moriya interactions and discover a broad region in the zero-temperature phase diagram which hosts quantum skyrmion lattices. We argue that the quantum skyrmion lattice phase can be…
Spin-polarized scanning tunneling microscopy (SPSTM) was used to directly image nanoscale Néel skyrmions in a SrIrO3 / SrRuO3 bilayer system that are among the smallest reported to date in any system. Off-axis magnetron sputtering was used to cap epitaxial films of the oxide ferromagnet SRO with 2 unit cells of SrIrO3, intended to provide interfacial spin orbit coupling. Atomic resolution STM imaging and tunneling spectroscopy were used to identify island-like SrIrO3 grains and small regions of bare SrRuO3. Isolated skyrmions were only observed in SrIrO3-covered regions of the film, and exhibi…
The transport response of dipole skyrmions in amorphous centrosymmetric Fe/Gd multilayer is investigated by temperature and field-dependent resistivity measurements collected in three current and magnetic field configurations. It is shown that a dipole skyrmion lattice phase may form at certain temperatures leading to a unique signature of the polar longitudinal resistivity. This signature differs from the conventional field-varying parabolic response associated with stripe phases, which transition to a disordered skyrmion phase under applied fields. Transport measurements under different fiel…
The skyrmions generated by frustration in centrosymmetric structures host extra internal degrees of freedom: vorticity and helicity, resulting in distinctive properties and potential functionality, which are not shared by the skyrmions stemming from the Dzyaloshinskii-Moriya interaction in noncentrosymmetric structures. The present work indicates that the magnetism-driven electric polarization carried by skyrmions provides a direct handle for tuning helicity. Especially for the in-plane magnetized skyrmions, the helicity can be continuously rotated and exactly picked by applying an external el…
Realizing topological magnetism and its electric control are intensive topics in the spintronics due to their promising applications in information storage and logic technologies. Here we unveil that both can be achieved in the two-dimensional (2D) magnetoelectric multiferroics. Using first-principles calculations, we show that strong Dzyaloshinskii-Moriya interaction (DMI), which is the key ingredient for the formation of exotic chiral magnetism, could be induced in 2D multiferroics with vertical electric polarization via Rashba effect. We verify that such significant DMI can promote sub-10 n…
When spin polarised electrons flow through a magnetic texture a transfer torque is generated. We examine the effect of this torque on skyrmions and skyrmion bags, skyrmionic structures of arbitrary integer topological degree, in thin ferromagnetic films. Using micromagnetic simulations and analysis from the well known Thiele equation we explore the potential for sorting or binning skyrmions of varying degrees mechanically. We investigate the applicability of the Thiele equation to problems of this nature and derive a theory of skyrmion deflection ordered by topological degree.
Odd-angular momentum exciton states are dark to light in monolayers of transition-metal dichalcogenides and can be addressed only by two-photon probes. Besides, $2p$ excitons states are expected to show a fine splitting that arises from the peculiar electronic band structure of the material, characterized by a finite Berry curvature around each valley. In this work we study in detail the coupling of photons to $p$ exciton states and we find that the Rashba spin-orbit interaction or a Skyrmion in the transition-metal dichalcogenide substrate can be exploited to engineer finite optical selection…
Ultrafast manipulation of magnetic skyrmions by microwave fields
School of Materials and Physics, China University of Mining and Technology（中国矿业大学材料科学与工程学院）；Center for Quantum Matter, School of Physics, Zhejiang University（浙江大学物理学院量子物质研究中心）
We show that properly engineered amorphous Fe-Gd alloy thin films with perpendicular magnetic anisotropy exhibit room-temperature skyrmion molecules, or a pair of like-polarity, opposite-helicity skyrmions. Magnetic mirror symmetry planes present in the stripe phase, instead of chiral exchange, determine the internal skyrmion structure and the net achirality of the skyrmion phase. Our study shows that stripe domain engineering in amorphous alloy thin films may enable the creation of skyrmion phases with technologically desirable properties.
A magnetic skyrmionium is a nontopological soliton, which has a doughnut-like out-of-plane spin texture in thin films, and can be phenomenologically viewed as a coalition of two topological magnetic skyrmions with opposite topological numbers. Due to its zero topological number ($Q=0$) and doughnut-like structure, the skyrmionium has its distinctive characteristics as compared to the skyrmion with $Q=\pm 1$. Here we systematically study the generation, manipulation and motion of a skyrmionium in ultrathin magnetic nanostructures by applying a magnetic field or a spin-polarized current. It is f…
Magnetic skyrmions are chiral nanoscale spin textures which are usually induced by Dzyaloshinskii-Moriya interaction (DMI). Recently, magnetic skyrmions have been observed in two-dimensional (2D) van der Waals (vdW) ferromagnetic materials, such as Fe$_{3}$GeTe$_{2}$. The electric control of skyrmions is important for their potential application in low-power memory technologies. Here, we predict that DMI and magnetic skyrmions in a Fe$_{3}$GeTe$_{2}$ monolayer can be controlled by ferroelectric polarization of an adjacent 2D vdW ferroelectric In$_{2}$Se$_{3}$. Based on density functional theor…
Magnetic skyrmions, which are topologically distinct magnetic spin textures, are gaining increased attention for their unique physical properties and potential applications in spintronic devices. Here we present a design strategy for skyrmion host candidates based on combinations of magnetic spin, asymmetric building units having stereo-active lone-pair electrons, and polar lattice symmetry. To demonstrate the viability of the proposed rational design principles, we successfully synthesized Fe(IO3)3 polycrystalline sample and single crystals by using a new simplified low-temperature pathway, w…
Topologically nontrivial field configurations called "baby skyrmions" behave like particles and give origins to the field of skyrmionics that promises racetrack memory and other technological applications. Unraveling the non-equilibrium behavior of such topological solitons is a challenge. We realize baby skyrmions in a chiral liquid crystal and, using numerical modeling and polarized video microscopy, demonstrate electrically driven squirming motion. We reveal the intricate details of non-equilibrium topology-preserving textural changes driving this behavior. Direction of the skyrmion's motio…
Based on a combined charge and vector spin transport theory capable of imaging noncollinear magnetic textures on surfaces with spin-polarized scanning tunneling microscopy (SP-STM), the high-resolution tunneling electron charge and coupled spin transport properties of a variety of Néel- and Bloch-type skyrmions are investigated. Axially symmetric skyrmions are considered within the same topology class characterized by a vorticity value of $m=1$, and their helicities are varied by taking $γ=0$ and $π$ values for the Néel skyrmions and $γ=-π/2$ and $π/2$ values for the Bloch skyrmions. Depending…
When magnetic skyrmions are moved via currents, they do not strictly travel along the path of the current, instead their motion also gains a transverse component. This so-called skyrmion Hall effect can be detrimental in potential skyrmion devices because it drives skyrmions towards the edge of their hosting material where they face potential annihilation. Here we experimentally modify a skyrmion model system - an atomic Pd/Fe bilayer on Ir(111) - by decorating the film edge with ferromagnetic Co/Fe patches. Employing spin-polarized scanning tunneling microscopy, we demonstrate that this ferro…
Magnetic skyrmions, as a whirling spin texture with axisymmetry, cannot be propelled by a uniform magnetic field. Therefore, reported skyrmion motions have been induced using other sorts of stimuli; typically, electric currents in magnetic metals as well as spin waves, thermal gradient, and field gradient have manifested their ability to drive skyrmion motion. Here, we demonstrate, through micromagnetic simulations and analytically, that magnetic skyrmions can be displaced by a uniform perpendicular magnetic field via a domain-wall (DW) mediator. For a fixed field strength, the velocity of a s…
