Origin of skyrmion lattice phase splitting in Zn-substituted Cu$_{2}$OSeO$_{3}$
A. Štefančič, S. Moody, T. J. Hicken, T. M. Birch, G. Balakrishnan, S. A. Barnett, M. Crisanti, J. S. O. Evans, S. J. R. Holt, K. J. A. Franke, P. D. Hatton, B.… 展开作者
A. Štefančič, S. Moody, T. J. Hicken, T. M. Birch, G. Balakrishnan, S. A. Barnett, M. Crisanti, J. S. O. Evans, S. J. R. Holt, K. J. A. Franke, P. D. Hatton, B. M. Huddart, M. R. Lees, F. L. Pratt, C. C. Tang, M. N. Wilson, F. Xiao, T. Lancaster
备注：
5 pages, 6 figures, includes supplemental material
We present an investigation into the structural and magnetic properties of Zn-substituted Cu$_{2}$OSeO$_{3}$, a system in which the skyrmion lattice (SkL) phase in the magnetic field-temperature phase diagram was previously seen to split as a function of increasing Zn concentration. We find that splitting of the SkL is only observed in polycrystalline samples and reflects the occurrence of several coexisting phases with different Zn content, each distinguished by different magnetic behaviour. No such multiphase behaviour is observed in single crystal samples.
We report small angle X-ray scattering (SAXS) measurements of the skyrmion lattice in two 200~nm thick Cu$_2$OSeO$_3$ lamellae aligned with the applied magnetic field parallel to the out of plane [110] or [100] crystallographic directions. Our measurements show that the equilibrium skyrmion phase in both samples is expanded significantly compared to bulk crystals, existing between approximately 30 and 50~K over a wide region of magnetic field. This skyrmion state is elliptically distorted at low fields for the [110] sample, and symmetric for the [100] sample, possibly due to crystalline anisot…
Skyrmions in confined geometries have been a subject of increasing interest due to the different properties that they exhibit compared to their bulk counterparts. In this study, nanoparticles of skyrmion-hosting $\text{Cu}_{2}\text{OSeO}_{3}$ have been synthesised using a precipitation method followed by thermal treatment. This enables us to produce nanoparticles whose mean size varies from tens of nanometers to a few micrometers by varying the temperature and duration of the thermal decomposition of the precursor. These sizes span the $\sim 63$~nm diameter of skyrmions in $\text{Cu}_{2}\text{…
We present long-wavelength neutron diffraction data measured on both single crystal and polycrystalline samples of the skyrmion host material Cu$_{2}$OSeO$_{3}$. We observe magnetic satellites around the $(0\bar{1}1)$ diffraction peak not accessible to other techniques, and distinguish helical from conical spin textures in reciprocal space. We confirm successive transitions from helical to conical to field polarised ordered spin textures as the external magnetic field is increased. The formation of a skyrmion lattice with propagation vectors perpendicular to the field direction is observed in …
Skyrmions are nanometric spin whirls that can be stabilized in magnets lacking inversion symmetry. The properties of isolated skyrmions embedded in a ferromagnetic background have been intensively studied. We show that single skyrmions and clusters of skyrmions can also form in the helical phase and investigate theoretically their energetics and dynamics. The helical background provides natural one-dimensional channels along which a skyrmion can move rapidly. In contrast to skyrmions in ferromagnets, the skymion-skyrmion interaction has a strong attractive component and thus skyrmions tend to …
Chiral magnetic textures with non-trivial topology are known as skyrmions, and due to their unique properties they are promising in novel magnetic storage applications. While the electric manipulation of either isolated skyrmions or a whole skyrmion lattice have been intensively reported, the electric effects on skyrmion clusters remain scarce. In magnetoelectric compound Cu$_2$OSeO$_3$, a skyrmion cluster can be created near the helical-skyrmion phase boundary. Here, we report the in situ electric field writing/erasing of skyrmions in such a skyrmion cluster. Our real space/time image data ob…
We report small angle neutron scattering (SANS) measurements of the skyrmion lattice in (Cu$_{0.976}$Zn$_{0.024}$)$_2$OSeO$_3$ under the application of an electric field. These measurements show an expansion of the skyrmion lattice stability region with electric field similar to that seen in pristine Cu$_2$OSeO$_3$. Furthermore, using time-resolved SANS, we observe the slow formation of skyrmions after an electric or magnetic field is applied, which has not been observed in pristine Cu$_2$OSeO$_3$ crystals. The measured formation times are dramatically longer than the corresponding skyrmion de…
Magnetic skyrmions, a topologically stable spin swirling object, have attracted a great interest due to their potential applications in future spintronics and ultra high dense magnetic memory devices. Cu$_2$OSeO$_3$ is only known insulating chiral helimagnet with multiple phases including skyrmion phase. Existence of skyrmion phase as well as first and second order phase transitions make Cu$_2$OSeO$_3$ a promissing candidate for investigating complex magnetic phenomena. Here, we report that both first and second order magnetic phase transitions are responsible in determining the phase diagram …
Magnetic skyrmions are localized nanometric spin textures with quantized winding numbers as the topological invariant. Rapidly increasing attention has been paid to the investigations of skyrmions since their experimental discovery in 2009, due both to the fundamental properties and the promising potential in spintronics based applications. However, controlled creation of skyrmions remains a pivotal challenge towards technological applications. Here, we report that skyrmions can be created locally by electric field in the magnetoelectric helimagnet Cu$\mathsf{_2}$OSeO$\mathsf{_3}$. Using Loren…
The Effects of Cobalt Doping on the Skyrmion Hosting Material Cu$_2$OSeO$_3$
The University of Auckland（奥克兰大学）；MacDiarmid Institute for Advanced Materials and Nanotechnology（麦克迪亚米德先进材料与纳米技术研究所）；Australian Institute of Nuclear Science and Engineering（澳大利亚核科学与工程研究所）；University of Fribourg（弗里堡大学）；Australian Centre for Neutron Scattering, ANSTO（澳大利亚中子散射中心，澳大利亚核科学与技术组织）；University of New South Wales（新南威尔士大学）
The manifestation of skyrmions in the Mott-insulator Cu$_2$OSeO$_3$ originates from a delicate balance between magnetic and electronic energy scales. As a result of these intertwined couplings, the two symmetry-inequivalent magnetic ions, Cu-I and Cu-II, bond into a spin S=1 entangled tetrahedron. However, conceptualizing the unconventional properties of this material and the energy of the competing interactions is a challenging task due the complexity of this system. Here we combine X-ray Absorption Spectroscopy and Resonant Inelastic X-ray Scattering to uncover the electronic and magnetic ex…
The cubic chiral helimagnets with the $P2_13$ space group represent a group of compounds in which the stable skyrmion-lattice state is experimentally observed. The key parameter that controls the energy landscape of such systems and determines the emergence of a topologically nontrivial magnetic structures is the Dzyaloshinskii-Moriya interaction (DMI). Chemical substitution is recognized as a convenient instrument to tune the DMI in real materials and has been successfully utilized in studies of a number of chiral magnets, such as MnSi, FeGe, MnGe, and others. In our study, we applied small-a…
Magnetic skyrmions are nano-sized topological spin textures stabilized by a delicate balance of magnetic energy terms. The chemical substitution of the underlying crystal structure of skyrmion-hosting materials offers a route to manipulate these energy contributions, but also introduces additional effects such as disorder and pinning. While the effects of doping and disorder have been well studied in B20 metallic materials such as Fe$_{1-x}$Co$_x$Si and Mn$_{1-x}$Fe$_x$Si, the consequences of chemical substitution in the magnetoelectric insulator Cu$_2$OSeO$_3$ have not been fully explored. In…
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…
Small angle neutron scattering measurements have been performed to study the thermodynamic stability of skyrmion-lattice phases in Cu$_2$OSeO$_3$. We found that the two distinct skyrmion-lattice phases [SkX(1) and SkX(2) phases] can be stabilized through different thermal histories; by cooling from the paramagnetic phase under finite magnetic field, the SkX(2) phase is selected. On the other hand, the 30$^{\circ}$-rotated SkX(1) phase becomes dominant by heating the sample from the ordered conical phase under finite field. This difference in stabilization is surprisingly similar to the irrever…
The strongly correlated cuprate Cu$_2$OSeO$_3$ has recently been identified as the first insulating system exhibiting a skyrmion lattice phase. Using a microscopic multi-boson theory for its magnetic ground state and excitations, we establish the presence of two distinct types of modes: a low energy manifold that includes a gapless Goldstone mode and a set of weakly dispersive high-energy magnons. These spectral features are the most direct signatures of the fact that the essential magnetic building blocks of Cu$_2$OSeO$_3$ are not individual Cu spins, but rather weakly-coupled Cu$_4$ tetrahed…
Due to their topological protection and nanometric size, magnetic skyrmions are anticipated to form components of new high-density memory technologies. In metallic systems skyrmion manipulation is achieved easily under a low density electric current flow, although the inevitable thermal dissipation ultimately limits the energy efficacy of potential applications. On the other hand, a near dissipation-free skyrmion and skyrmion phase manipulation is expected by using electric \emph{fields}, thus meeting better the demands of an energy-conscious society. In this work on an insulating chiral magne…
Using small angle neutron scattering, we have investigated higher-order peaks in the skyrmion-lattice phase of Cu$_2$OSeO$_3$, in which two different skyrmion lattices, SkX1 and SkX2, are known to form. For each skyrmion-lattice phase, we observed two sets of symmetrically inequivalent peaks at the higher-order-reflection positions with the indices $(110)$ and $(200)$. Under the condition where the SkX1 and SkX2 coexist, we confirmed the absence of the scattering at $\mathbf{Q}$ positions combining reflections from the two phases, indicating a significantly weak double-scattering component. De…
We report studies of thermal conductivity as functions of magnetic field and temperature in the helimagnetic insulator Cu$_2$OSeO$_3$ that reveal novel features of the spin-phase transitions as probed by magnon heat conduction. The tilted conical spiral and low-temperature skyrmion phases, recently identified in small-angle neutron scattering studies, are clearly identified by sharp signatures in the magnon thermal conductivity. Magnon scattering associated with the presence of domain boundaries in the tilted conical phase and regions of skyrmion and conical-phase coexistence are identified.
In this work, we present a comprehensive study of the low energy optical magnetic response of the skyrmionic Mott insulator Cu$_2$OSeO$_3$ via high resolution time-domain THz spectroscopy. In zero field, a new magnetic excitation not predicted by spin-wave theory with frequency $f$ = 2.03 THz is observed and shown, with accompanying time-of-flight neutron scattering experiments, to be a zone folded magnon from the $\mathrm{R}$ to $\mathrmΓ$ points of the Brillouin zone. Highly sensitive polarimetry experiments performed in weak magnetic fields, $μ_0$H $<$ 200 mT, observe Faraday and Kerr rotat…
The Skyrme-particle, the $skyrmion$, was introduced over half a century ago and used to construct field theories for dense nuclear matter. But with skyrmions being mathematical objects - special types of topological solitons - they can emerge in much broader contexts. Recently skyrmions were observed in helimagnets, forming nanoscale spin-textures that hold promise as information carriers. Extending over length-scales much larger than the inter-atomic spacing, these skyrmions behave as large, classical objects, yet deep inside they are of quantum origin. Penetrating into their microscopic root…
We present an investigation of the magnetic field-temperature phase diagram of Cu$_2$OSeO$_3$ based on DC magnetisation and AC susceptibility measurements covering a broad frequency range of four orders of magnitude, from very low frequencies reaching 0.1 Hz up to 1 kHz. The experiments were performed in the vicinity of $T_C=58.2$ K and around the skyrmion lattice A-phase. At the borders between the different phases the characteristic relaxation times reach several milliseconds and the relaxation is non-exponential. Consequently the borders between the different phases depend on the specific c…
We propose a skyrmion liquid state for the non-Fermi liquid (NFL) phase in Ge-substituted YbRh$_{2}$Si$_{2}$, where skyrmions form their Fermi surface, argued to result from the strongly coupled nature between skyrmions and itinerant electrons. The fermionized skyrmion theory identifies the antiferromagnetic (AF) transition with the Lifshitz transition, where the quantum critical point (QCP) is characterized by the dynamical critical exponent $z = 2$. Nonlocal interactions between skyrmions allow a critical line above the AF QCP, which originates from the Kondo-coupling effect with itinerant e…
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.
The skyrmion is a topologically stable spin texture, in which the spin direction wraps a sphere. The topological nature gives rise to emergent electromagnetic phenomena such as topological Hall effect. Recently, the crystallization of nanoscale skyrmions was observed in chiral helimagnets with use of the neutron diffraction and Lorentz transmission electron microscopy. The skyrmions are quite mobile under electric current density as low as $\sim$ 10$^6$ A/m$^2$, and, in some cases, stable up to near room temperature. These features suggest that the skyrmions may work as a magnetic stable-varia…
We present longitudinal-field muon-spin relaxation (LF $μ$SR) measurements on two systems that stabilize a skyrmion lattice (SkL): Cu$_2$OSeO$_3$, and Co$_x$Zn$_y$Mn$_{20-x-y}$ for $(x,y)~=~(10,10)$, $(8,9)$ and $(8,8)$. We find that the SkL phase of Cu$_2$OSeO$_3$ exhibits emergent dynamic behavior at megahertz frequencies, likely due to collective excitations, allowing the SkL to be identified from the $μ$SR response. From measurements following different cooling protocols and calculations of the muon stopping site, we suggest that the metastable SkL is not the majority phase throughout the …
A Surface-confined Spiral State With the Double Period in the Cubic Chiral Helimagnet Cu$_2$OSeO$_3$
The University of Tokyo（东京大学）；Paul Scherrer Institute (PSI)（保罗谢勒研究所）；École Polytechnique Fédérale de Lausanne (EPFL)（洛桑联邦理工学院）；Institute for Basic Science（基础科学研究所）；Durham University（杜伦大学）；Rutherford Appleton Laboratory（卢瑟福·阿普尔顿实验室）；ALBA Synchrotron Light Source（阿尔巴同步辐射光源）；Institut Laue–Langevin（朗之万研究所）
We show that continuous and spin-lattice models of chiral ferro- and antiferromagnets provide the existence of an infinite number of stable soliton solutions of any integer topological charge. A detailed description of the morphology of new skyrmions and the corresponding energy dependencies are provided. The considered model is general, and is expected to predict a plethora of particle-like states which may occur in various chiral magnets including atomic layers, e.g., PdFe/Ir(111), rhombohedral GaV$_4$S$_8$ semiconductor, B20-type alloys as Mn$_{1-x}$Fe$_x$Ge, Mn$_{1-x}$Fe$_x$Si, Fe$_{1-x}$C…
We have used inelastic neutron scattering to measure the magnetic excitation spectrum along the high-symmetry directions of the first Brillouin zone of the magnetic skyrmion hosting compound Cu$_2$OSeO$_3$. The majority of our scattering data are consistent with the expectations of a recently proposed model for the magnetic excitations in Cu$_2$OSeO$_3$, and we report best-fit parameters for the dominant exchange interactions. Important differences exist, however, between our experimental findings and the model expectations. These include the identification of two energy scales that likely ari…
Skyrmions are twirling magnetic textures whose non-trivial topology leads to particle-like properties promising for information technology applications. Perhaps the most important aspect of interacting particles is their ability to form thermodynamically distinct phases from gases and liquids to crystalline solids. Dilute gases of skyrmions have been realized in artificial multilayers, and solid crystalline skyrmion lattices have been observed in bulk skyrmion hosting materials. Yet, to date melting of the skyrmion lattice into a skyrmion liquid has not been reported experimentally. Through di…
Previous observations of metastable magnetic skyrmions have shown that close to the equilibrium pocket the metastable state has a short lifetime, and therefore rapid cooling is required to generate a significant skyrmion population at low temperatures. Here, we report that the lifetime of metastable skyrmions in Cu$_2$OSeO$_3$ is extended by a factor of 50 with the introduction of only 2.5% zinc doping, allowing over 50% of the population to survive when field-cooling at a rate of just 1 K/min. Our systematic study suggests that the lifetime enhancement is due to the removal of spins by the no…
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…
Magnetic skyrmions are nano-sized topologically protected spin textures with particle-like properties. They can form lattices perpendicular to the magnetic field and the orientation of these skyrmion lattices with respect to the crystallographic lattice is governed by spin-orbit coupling. By performing small angle neutron scattering measurements, we investigate the coupling between the crystallographic and skyrmion lattices in both Cu$_2$OSeO$_3$ and the archetype chiral magnet MnSi. The results reveal that the orientation of the skyrmion lattice is primarily determined by the magnetic field d…
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…
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 $q \paralle…
Magnetic materials can host skyrmions, which are topologically non-trivial spin textures. In chiral magnets with cubic lattice symmetry, all previously-observed skyrmion phases require thermal fluctuations to become thermodynamically stable in bulk materials, and therefore exist only at relatively high temperature, close to the helimagnetic transition temperature. Other stabilization mechanisms require a lowering of the cubic crystal symmetry. Here, we report the identification of a second skyrmion phase in Cu$_{2}$OSeO$_{3}$ at low temperature and in the presence of an applied magnetic field.…
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…
The chiral magnet Cu$_{2}$OSeO$_{3}$ hosts a skyrmion lattice, that may be equivalently described as a superposition of plane waves or lattice of particle-like topological objects. A thermal gradient may break up the skyrmion lattice and induce rotating domains raising the question which of these scenarios better describes the violent dynamics at the domain boundaries. Here we show that in an inhomogeneous temperature gradient caused by illumination in a Lorentz Transmission Electron Microscope different parts of the skyrmion lattice can be set into motion with different angular velocities. Tr…
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 $\l…
We present a theoretical examination of the magneto-electric response in the recently discovered multiferroic insulator Cu$_2$OSeO$_3$. Combining Monte Carlo simulation and Ginzburg-Landau analysis we predict the response in each of the magnetic phases, including helical, conical, ferromagnetic and Skyrmion crystal phases, both for thin film and bulk systems. A common feature for all non-collinear phases is that the magneto-electric susceptibility increases linearly with the applied magnetic field. Being both calculable and measurable, the magneto-electric susceptibility can serve as a new pow…
We present an investigation of the influence of low-levels of chemical substitution on the magnetic ground state and N{\' e}el skyrmion lattice (SkL) state in GaV$_4$S$_{8-y}$Se$_y$, where $y =0, 0.1, 7.9$, and $8$. Muon-spin spectroscopy ($μ$SR) measurements on $y=0$ and 0.1 materials reveal the magnetic ground state consists of microscopically coexisting incommensurate cycloidal and ferromagnetic environments, while chemical substitution leads to the growth of localized regions of increased spin density. $μ$SR measurements of emergent low-frequency skyrmion dynamics show that the SkL exists …
