Topological aspects of multi-kantiferromagnetism in cubic rare-earth compounds.

We advertise rare-earth intermetallics with high-symmetry crystal structures and competing interactions as a possible materials platform hosting spin structures with non-trivial topological properties. Focusing on the series of cubicRCu compounds, whereR= Ho, Er, Tm, the bulk properties of these systems display exceptionally rich magnetic phase diagrams hosting an abundance of different phase pockets characteristic of antiferromagnetic order in the presence of delicately balanced interactions. The electrical transport properties exhibit large anomalous contributions suggestive of topologically non-trivial winding in the electronic and magnetic structures. Neutron diffraction identifies spontaneous long-range magnetic order in terms of commensurate and incommensurate variations of(ππ0)antiferromagnetism with the possibility for various multi-kconfigurations. Motivated by general trends in these materials, we discuss the possible existence of topologically non-trivial winding in real and reciprocal space in the class ofRCu compounds including antiferromagnetic skyrmion lattices. Putatively bringing together different limits of non-trivial topological winding in the same material, the combination of properties inRCu systems promises access to advanced functionalities.

Topological magnon band structure of emergent Landau levels in a skyrmion lattice.

The motion of a spin excitation across topologically nontrivial magnetic order exhibits a deflection that is analogous to the effect of the Lorentz force on an electrically charged particle in an orbital magnetic field. We used polarized inelastic neutron scattering to investigate the propagation of magnons (i.e., bosonic collective spin excitations) in a lattice of skyrmion tubes in manganese silicide. For wave vectors perpendicular to the skyrmion tubes, the magnon spectra are consistent with the formation of finely spaced emergent Landau levels that are characteristic of the fictitious magnetic field used to account for the nontrivial topological winding of the skyrmion lattice. This provides evidence of a topological magnon band structure in reciprocal space, which is borne out of the nontrivial real-space topology of a magnetic order.

Optimized signal deduction procedure for the MIEZE spectroscopy technique.

A method is reported to determine the phase and amplitude of sinusoidally modulated event rates, binned into four bins per oscillation, based on data generated at the resonant neutron spin-echo spectrometer RESEDA at FRM-II. The presented algorithm relies on a reconstruction of the unknown parameters. It omits a calculation-intensive fitting procedure and avoids contrast reduction due to averaging effects. It allows the current data acquisition bottleneck at RESEDA to be relaxed by a factor of four and thus increases the potential time resolution of the detector by the same factor. The approach is explained in detail and compared with the established fitting procedures of time series having four and 16 time bins per oscillation. In addition the empirical estimates of the errors of the three methods are presented and compared with each other. The reconstruction is shown to be unbiased, asymptotic and efficient for estimating the phase. Reconstructing the contrast increases the error bars by roughly 10% as compared with fitting 16 time-binned oscillations. Finally, the paper gives heuristic, analytical equations to estimate the error for phase and contrast as a function of their initial values and counting statistics.

Ferromagnetic Resonance with Magnetic Phase Selectivity by Means of Resonant Elastic X-Ray Scattering on a Chiral Magnet.

Cubic chiral magnets, such as Cu_{2}OSeO_{3}, exhibit a variety of noncollinear spin textures, including a trigonal lattice of spin whirls, the so-called skyrmions. Using magnetic resonant elastic x-ray scattering (REXS) on a crystalline Bragg peak and its magnetic satellites while exciting the sample with magnetic fields at gigahertz frequencies, we probe the ferromagnetic resonance (FMR) modes of these spin textures by means of the scattered intensity. Most notably, the three eigenmodes of the skyrmion lattice are detected with large sensitivity. As this novel technique, which we label REXS FMR, is carried out at distinct positions in reciprocal space, it allows us to distinguish contributions originating from different magnetic states, providing information on the precise character, weight, and mode mixing as a prerequisite of tailored excitations for applications.

Unique Crystal Structure of Ca_{2}RuO_{4} in the Current Stabilized Semimetallic State.

The electric-current stabilized semimetallic state in the quasi-two-dimensional Mott insulator Ca_{2}RuO_{4} exhibits an exceptionally strong diamagnetism. Through a comprehensive study using neutron and x-ray diffraction, we show that this nonequilibrium phase assumes a crystal structure distinct from those of equilibrium metallic phases realized in the ruthenates by chemical doping, high pressure, and epitaxial strain, which in turn leads to a distinct electronic band structure. Dynamical mean field theory calculations based on the crystallographically refined atomic coordinates and realistic Coulomb repulsion parameters indicate a semimetallic state with partially gapped Fermi surface. Our neutron diffraction data show that the nonequilibrium behavior is homogeneous, with antiferromagnetic long-range order completely suppressed. These results provide a new basis for theoretical work on the origin of the unusual nonequilibrium diamagnetism in Ca_{2}RuO_{4}.

Compact susceptometer for studies under transverse field geometries at very low temperatures.

We present the design of a compact AC susceptometer for studies under arbitrarily oriented static magnetic fields, in particular magnetic fields oriented transverse to the AC excitation field. The small size of the susceptometer permits versatile use in conventional cryostats with superconducting magnet systems. The design of the susceptometer minimizes parasitic signal contributions while providing excellent thermal anchoring suitable for measurements in a wide range down to very low temperatures. The performance is illustrated by means of measurements of the transverse susceptibility at the magnetic field tuned quantum phase transition of the dipolar-coupled Ising ferromagnet LiHoF4.

Ultrasmall Moment Incommensurate Spin Density Wave Order Masking a Ferromagnetic Quantum Critical Point in NbFe_{2}.

In the metallic magnet Nb_{1-y}Fe_{2+y}, the low temperature threshold of ferromagnetism can be investigated by varying the Fe excess y within a narrow homogeneity range. We use elastic neutron scattering to track the evolution of magnetic order from Fe-rich, ferromagnetic Nb_{0.981}Fe_{2.019} to approximately stoichiometric NbFe_{2}, in which we can, for the first time, characterize a long-wavelength spin density wave state burying a ferromagnetic quantum critical point. The associated ordering wave vector q_{SDW}=(0,0,l_{SDW}) is found to depend significantly on y and T, staying finite but decreasing as the ferromagnetic state is approached. The phase diagram follows a two-order-parameter Landau theory, for which all of the coefficients can now be determined. Our findings suggest that the emergence of spin density wave order cannot be attributed to band structure effects alone. They indicate a common microscopic origin of both types of magnetic order and provide strong constraints on related theoretical scenarios based on, e.g., quantum order by disorder.

Response of the Skyrmion Lattice in MnSi to Cubic Magnetocrystalline Anisotropies.

We report high-precision small-angle neutron scattering of the orientation of the Skyrmion lattice in a spherical sample of MnSi under systematic changes of the magnetic field direction. For all field directions the Skyrmion lattice may be accurately described as a triple-Q[over →] state, where the modulus |Q[over →]| is constant and the wave vectors enclose rigid angles of 120°. Along a great circle across ⟨100⟩, ⟨110⟩, and ⟨111⟩ the normal to the Skyrmion-lattice plane varies systematically by ±3° with respect to the field direction, while the in-plane alignment displays a reorientation by 15° for magnetic field along ⟨100⟩. Our observations are qualitatively and quantitatively in excellent agreement with an effective potential, which is determined by the symmetries of the tetrahedral point group T and includes contributions up to sixth order in spin-orbit coupling, providing a full account of the effect of cubic magnetocrystalline anisotropies on the Skyrmion lattice in MnSi.

Manipulation of skyrmion motion by magnetic field gradients.

Magnetic skyrmions are particle-like, topologically protected magnetisation entities that are promising candidates as information carriers in racetrack memory. The transport of skyrmions in a shift-register-like fashion is crucial for their embodiment in practical devices. Here, we demonstrate that chiral skyrmions in Cu2OSeO3 can be effectively manipulated under the influence of a magnetic field gradient. In a radial field gradient, skyrmions were found to rotate collectively, following a given velocity-radius relationship. As a result of this relationship, and in competition with the elastic properties of the skyrmion lattice, the rotating ensemble disintegrates into a shell-like structure of discrete circular racetracks. Upon reversing the field direction, the rotation sense reverses. Field gradients therefore offer an effective handle for the fine control of skyrmion motion, which is inherently driven by magnon currents. In this scheme, no local electric currents are needed, thus presenting a different approach to shift-register-type operations based on spin transfer torque.

Determination of the hydrogen-bond network and the ferrimagnetic structure of a rockbridgeite-type compound, [Formula: see text].

Applying neutron powder diffraction, four unique hydrogen positions were determined in a rockbridgeite-type compound, [Formula: see text] [Formula: see text]. Its honeycomb-like H-bond network running without interruption along the crystallographic [Formula: see text] axis resembles those in alkali sulphatic and arsenatic oxyhydroxides. They provide the so-called dynamically disordered H-bond network over which protons are superconducting in a vehicle mechanism. This is indicated by dramatic increases of dielectric constant and loss factor at room temperature. The relevance of static and dynamic disorder of OH and HOH groups are explained in terms of a high number of structural defects at octahedral chains alternatingly half-occupied by [Formula: see text] cations. The structure is built up by unusual octahedral doublet, triplet, and quartet clusters of aliovalent 3d transition metal cations, predicting complicate magnetic ordering and interaction. The ferrimagnetic structure below the Curie temperature [Formula: see text]-83 K could be determined from the structure analysis with neutron diffraction data at 25 K.

Linearly polarized GHz magnetization dynamics of spin helix modes in the ferrimagnetic insulator Cu2OSeO3.

Linear dichroism - the polarization dependent absorption of electromagnetic waves- is routinely exploited in applications as diverse as structure determination of DNA or polarization filters in optical technologies. Here filamentary absorbers with a large length-to-width ratio are a prerequisite. For magnetization dynamics in the few GHz frequency regime strictly linear dichroism was not observed for more than eight decades. Here, we show that the bulk chiral magnet Cu2OSeO3 exhibits linearly polarized magnetization dynamics at an unexpectedly small frequency of about 2 GHz at zero magnetic field. Unlike optical filters that are assembled from filamentary absorbers, the magnet is shown to provide linear polarization as a bulk material for an extremely wide range of length-to-width ratios. In addition, the polarization plane of a given mode can be switched by 90° via a small variation in width. Our findings shed a new light on magnetization dynamics in that ferrimagnetic ordering combined with antisymmetric exchange interaction offers strictly linear polarization and cross-polarized modes for a broad spectrum of sample shapes at zero field. The discovery allows for novel design rules and optimization of microwave-to-magnon transduction in emerging microwave technologies.

Dynamical Defects in Rotating Magnetic Skyrmion Lattices.

The chiral magnet Cu_{2}OSeO_{3} hosts a Skyrmion lattice that may be equivalently described as a superposition of plane waves or a lattice of particlelike topological objects. A thermal gradient may break up the Skyrmion lattice and induce rotating domains, raising the question of 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. Tracking the time dependence, we show that the constant rearrangement of domain walls is governed by dynamic 5-7 defects arranging into lines. An analysis of the associated defect density is described by Frank's equation and agrees well with classical 2D Monte Carlo simulations. Fluctuations of boundaries show a surgelike rearrangement of Skyrmion clusters driven by defect rearrangement consistent with simulations treating Skyrmions as point particles. Our findings underline the particle character of the Skyrmion.

Room-temperature helimagnetism in FeGe thin films.

Chiral magnets are promising materials for the realisation of high-density and low-power spintronic memory devices. For these future applications, a key requirement is the synthesis of appropriate materials in the form of thin films ordering well above room temperature. Driven by the Dzyaloshinskii-Moriya interaction, the cubic compound FeGe exhibits helimagnetism with a relatively high transition temperature of 278 K in bulk crystals. We demonstrate that this temperature can be enhanced significantly in thin films. Using x-ray scattering and ferromagnetic resonance techniques, we provide unambiguous experimental evidence for long-wavelength helimagnetic order at room temperature and magnetic properties similar to the bulk material. We obtain α intr = 0.0036 ± 0.0003 at 310 K for the intrinsic damping parameter. We probe the dynamics of the system by means of muon-spin rotation, indicating that the ground state is reached via a freezing out of slow dynamics. Our work paves the way towards the fabrication of thin films of chiral magnets that host certain spin whirls, so-called skyrmions, at room temperature and potentially offer integrability into modern electronics.

Reentrant Phase Diagram of Yb_{2}Ti_{2}O_{7} in a ⟨111⟩ Magnetic Field.

We present a magnetic phase diagram of rare-earth pyrochlore Yb_{2}Ti_{2}O_{7} in a ⟨111⟩ magnetic field. Using heat capacity, magnetization, and neutron scattering data, we show an unusual field dependence of a first-order phase boundary, wherein a small applied field increases the ordering temperature. The zero-field ground state has ferromagnetic domains, while the spins polarize along ⟨111⟩ above 0.65 T. A classical Monte Carlo analysis of published Hamiltonians does account for the critical field in the low T limit. However, this analysis fails to account for the large bulge in the reentrant phase diagram, suggesting that either long-range interactions or quantum fluctuations govern low field properties.

Ultra-high vacuum compatible preparation chain for intermetallic compounds.

We report the development of a versatile material preparation chain for intermetallic compounds, which focuses on the realization of a high-purity growth environment. The preparation chain comprises an argon glovebox, an inductively heated horizontal cold boat furnace, an arc melting furnace, an inductively heated rod casting furnace, an optically heated floating-zone furnace, a resistively heated annealing furnace, and an inductively heated annealing furnace. The cold boat furnace and the arc melting furnace may be loaded from the glovebox by means of a load-lock permitting to synthesize compounds starting with air-sensitive elements while handling the constituents exclusively in an inert gas atmosphere. All furnaces are all-metal sealed, bakeable, and may be pumped to ultra-high vacuum. We find that the latter represents an important prerequisite for handling compounds with high vapor pressure under high-purity argon atmosphere. We illustrate the operational aspects of the preparation chain in terms of the single-crystal growth of the heavy-fermion compound CeNi2Ge2.

Ultra-high vacuum compatible induction-heated rod casting furnace.

We report the design of a radio-frequency induction-heated rod casting furnace that permits the preparation of polycrystalline ingots of intermetallic compounds under ultra-high vacuum compatible conditions. The central part of the system is a bespoke water-cooled Hukin crucible supporting a casting mold. Depending on the choice of the mold, typical rods have a diameter between 6 mm and 10 mm and a length up to 90 mm, suitable for single-crystal growth by means of float-zoning. The setup is all-metal sealed and may be baked out. We find that the resulting ultra-high vacuum represents an important precondition for processing compounds with high vapor pressures under a high-purity argon atmosphere up to 3 bars. Using the rod casting furnace, we succeeded to prepare large high-quality single crystals of two half-Heusler compounds, namely, the itinerant antiferromagnet CuMnSb and the half-metallic ferromagnet NiMnSb.

Multidomain Skyrmion Lattice State in Cu2OSeO3.

Magnetic skyrmions in chiral magnets are nanoscale, topologically protected magnetization swirls that are promising candidates for spintronics memory carriers. Therefore, observing and manipulating the skyrmion state on the surface level of the materials are of great importance for future applications. Here, we report a controlled way of creating a multidomain skyrmion state near the surface of a Cu2OSeO3 single crystal, observed by soft resonant elastic X-ray scattering. This technique is an ideal tool to probe the magnetic order at the L3 edge of 3d metal compounds giving an average depth sensitivity of ∼50 nm. The single-domain 6-fold-symmetric skyrmion lattice can be broken up into domains, overcoming the propagation directions imposed by the cubic anisotropy by applying the magnetic field in directions deviating from the major cubic axes. Our findings open the door to a new way to manipulate and engineer the skyrmion state locally on the surface or on the level of individual skyrmions, which will enable applications in the future.

Band Structure of Helimagnons in MnSi Resolved by Inelastic Neutron Scattering.

A magnetic helix realizes a one-dimensional magnetic crystal with a period given by the pitch length λh. Its spin-wave excitations-the helimagnons-experience Bragg scattering off this periodicity, leading to gaps in the spectrum that inhibit their propagation along the pitch direction. Using high-resolution inelastic neutron scattering, the resulting band structure of helimagnons was resolved by preparing a single crystal of MnSi in a single magnetic-helix domain. At least five helimagnon bands could be identified that cover the crossover from flat bands at low energies with helimagnons basically localized along the pitch direction to dispersing bands at higher energies. In the low-energy limit, we find the helimagnon spectrum to be determined by a universal, parameter-free theory. Taking into account corrections to this low-energy theory, quantitative agreement is obtained in the entire energy range studied with the help of a single fitting parameter.

Universal helimagnon and skyrmion excitations in metallic, semiconducting and insulating chiral magnets.

Nearly seven decades of research on microwave excitations of magnetic materials have led to a wide range of applications in electronics. The recent discovery of topological spin solitons in chiral magnets, so-called skyrmions, promises high-frequency devices that exploit the exceptional emergent electrodynamics of these compounds. Therefore, an accurate and unified quantitative account of their resonant response is key. Here, we report all-electrical spectroscopy of the collective spin excitations in the metallic, semiconducting and insulating chiral magnets MnSi, Fe1-xCoxSi and Cu2OSeO3, respectively, using broadband coplanar waveguides. By taking into account dipolar interactions, we achieve a precise quantitative modelling across the entire magnetic phase diagrams using two material-specific parameters that quantify the chiral and the critical field energy. The universal behaviour sets the stage for purpose-designed applications based on the resonant response of chiral magnets with tailored electric conductivity and an unprecedented freedom for an integration with electronics.

Uniaxial Pressure Dependence of Magnetic Order in MnSi.

We report comprehensive small angle neutron scattering measurements complemented by ac susceptibility data of the helical order, conical phase, and Skyrmion lattice phase (SLP) in MnSi under uniaxial pressures. For all crystallographic orientations uniaxial pressure favors the phase for which a spatial modulation of the magnetization is closest to the pressure axis. Uniaxial pressures as low as 1 kbar applied perpendicular to the magnetic field axis enhance the Skyrmion lattice phase substantially, whereas the Skyrmion lattice phase is suppressed for pressure parallel to the field. Taken together we present quantitative microscopic information on how strain couples to magnetic order in the chiral magnet MnSi.