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We report the development of a versatile material preparation chain for intermetallic compounds that focuses on the realization of a high-purity growth environment. The preparation chain comprises of 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 operational aspects of the preparation chain in terms of the single-crystal growth of the heavy-fermion compound CeNi2Ge2., Comment: 12 pages, 11 figures

We report a kinetic small angle neutron scattering study of the skyrmion lattice (SL) in MnSi. Induced by an oscillatory tilting of the magnetic field direction, the elasticity and relaxation of the SL along the magnetic field direction have been measured with microsecond resolution. For the excitation frequency of 325 Hz the SL begins to track the tilting motion of the applied magnetic field under tilting angles exceeding $\alpha_c$ > 0.4{\deg}. Empirically the associated angular velocity of the tilting connects quantitatively with the critical charge carrier velocity of approx. 0.1mm/s under current driven spin transfer torques, for which the SL unpins. In addition, a pronounced temperature dependence of the skyrmion motion is attributed to the variation of the skyrmion stiffness. Taken together our study highlights the power of kinetic small angle neutron scattering as a new experimental tool to explore, in a rather general manner, the elasticity and impurity pinning of magnetic textures across a wide parameter space without parasitic signal interferences due to ohmic heating or Oersted magnetic fields.

Outstanding crystalline perfection is a key requirement for the formation of new forms of electronic order in a vast number of widely different materials. Whereas excellent sample quality represents a standard claim in the literature, there are, quite generally, no reliable microscopic probes to establish the nature and concentration of lattice defects such as voids, dislocations and different species of point defects on the level relevant to the length and energy scales inherent to these new forms of order. Here we report an experimental study of the archetypical skyrmion-lattice compound MnSi, where we relate the characteristic types of point defects and their concentration to the magnetic properties by combining different types of positron spectroscopy with ab-initio calculations and bulk measurements. We find that Mn antisite disorder broadens the magnetic phase transitions and lowers their critical temperatures, whereas the skyrmion lattice phase forms for all samples studied underlining the robustness of this topologically non-trivial state. Taken together, this demonstrates the unprecedented sensitivity of positron spectroscopy in studies of new forms of electronic order., Comment: 8 pages, 4 figures

We propose the design of a Resonance SPin-echo spECtrometer for exTreme studies, RESPECT, that is ideally suited for the exploration of non-dispersive processes such as diffusion, crystallization, slow dynamics, tunneling processes, crystal electric field excitations, and spin fluctuations. It is a variant of the conventional neutron spin-echo technique (NSE) by i) replacing the long precession coils by pairs of longitudinal neutron spin-echo coils combined with RF-spin flippers and ii) by stabilizing the neutron polarization with small longitudinal guide fields that can in addition be used as field subtraction coils thus allowing to adjust the field integrals over a range of 8 orders of magnitude. Therefore, the dynamic range of RESPECT can in principle be varied over 8 orders of magnitude in time, if neutrons with the required energy are made available. Similarly as for existing NSE-spectrometers, spin echo times of up to approximately 1 microsecond can be reached if the divergence and the correction elements are properly adjusted. Thanks to the optional use of neutron guides and the fact that the currents for the correction coils are much smaller than in standard NSE, intensity gains of at least one order of magnitude are expected , making the concept of RESPECT also competitive for operation at medium flux neutron sources. RESPECT can also be operated in a MIEZE configuration allowing the investigation of relaxation processes in depolarizing environments as they occur when magnetic fields are applied at the sample position, i.e. for the investigation of the dynamics of flux lines in superconductors, magnetic fluctuations in ferromagnetic materials, and samples containing hydrogen., Comment: 14 pages, 22 figures

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 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 bar. 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., Comment: 5 pages, 4 figures

We report the study of the skyrmion state near the surface of Cu$_2$OSeO$_3$ using soft resonant elastic x-ray scattering (REXS) at the Cu $L_3$ edge. Within the lateral sampling area of $200 \times 200$ $\mu$m$^2$, we found a long-range-ordered skyrmion lattice phase as well as the formation of skyrmion domains via the multiple splitting of the diffraction spots. In a recent REXS study of the skyrmion phase of Cu$_2$OSeO$_3$ [Phys. Rev. Lett. 112, 167202 (2014)], Langner et al. reported the observation of the unexpected existence of two distinct skyrmion sublattices that arise from inequivalent Cu sites, and that the rotation and superposition of the two periodic structures leads to a moir\'{e} pattern. However, we find no energy splitting of the Cu peak in x-ray absorption measurements and, instead, discuss alternative origins of the peak splitting. In particular, we find that for magnetic field directions deviating from the major cubic axes, a multidomain skyrmion lattice state is obtained, which consistently explains the splitting of the magnetic spots into two - and more - peaks., Comment: 6 pages, 3 figures

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 Cu$_{2}$OSeO$_{3}$ single crystal, observed by soft resonant elastic x-ray scattering. This technique is an ideal tool to probe the magnetic order at the $L_{3}$ edge of $3d$ metal compounds giving a depth sensitivity of ${\sim}50$ nm. The single-domain sixfold-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., Comment: 19 pages, 5 figures

The investigation of fragile and potentially inhomogeneous forms of ferromagnetic order under extreme conditions, such as low temperatures and high pressures, is of central interest for areas such as geophysics, correlated electron systems, as well as the optimization of materials synthesis for applications where particular material properties are required. We report neutron depolarization imaging measurements on the weak ferromagnet Ni$_3$Al under pressures up to 10kbar using a Cu:Be clamp cell. Using a polychromatic neutron beam with wavelengths $\lambda\geq$ 4\AA in combination with $^3$He neutron spin filter cells as polarizer and analyzer we were able to track differences of the pressure response in inhomogeneous samples by virtue of high resolution neutron depolarization imaging. This provides spatially resolved and non-destructive access to the pressure dependence of the magnetic properties of inhomogeneous ferromagnetic materials.

We report the magnetization, ac susceptibility, and specific heat of optically float-zoned single crystals of Fe$_{1-x}$Co$_{x}$Si, $0.20 \leq x \leq 0.50$. We determine the magnetic phase diagrams for all major crystallographic directions and cooling histories. After zero-field cooling, the phase diagrams resemble that of the archetypal stoichiometric cubic chiral magnet MnSi. Besides the helical and conical state, we observe a pocket of skyrmion lattice phase just below the helimagnetic ordering temperature. At the phase boundaries between these states evidence for slow dynamics is observed. When the sample is cooled in small magnetic fields, the phase pocket of skyrmion lattice may persist metastably down to lowest temperatures. Taken together with the large variation of the transition temperatures, transition fields, and the helix wavelength as a function of composition, this hysteresis identifies Fe$_{1-x}$Co$_{x}$Si as an ideal material for future experiments exploring, for instance, the topological unwinding of the skyrmion lattice., Comment: 14 pages, 11 figures

We report single crystal growth of the series of CeTAl$_3$ compounds with T = Cu, Ag, Au, Pd and Pt by means of optical float zoning. High crystalline quality was confirmed in a thorough characterization process. With the exception of CeAgAl$_3$, all compounds crystallize in the non-centrosymmetric tetragonal BaNiSn$_{3}$ structure (space group: I4mm, No. 107), whereas CeAgAl$_3$ adopts the related orthorhombic PbSbO$_2$Cl structure (Cmcm, No. 63). An attempt to grow CeNiAl$_3$ resulted in the composition CeNi$_2$Al$_5$. Low temperature resistivity measurements down to $\sim$0.1K did not reveal evidence suggestive of magnetic order in CePtAl$_3$ and CePdAl$_3$. In contrast, CeAuAl$_3$, CeCuAl$_3$ and CeAgAl$_3$ display signatures of magnetic transitions at 1.3K, 2.1K and 3.2K, respectively. This is consistent with previous reports of antiferromagnetic order in CeAuAl$_3$, and CeCuAl$_3$ as well as ferromagnetism in CeAgAl$_3$, respectively., Comment: 12 pages, 6 figures

Magnetic skyrmions are topologically non-trivial spin whirls that may not be transformed continuously into topologically trivial states such as ferromagnetic spin alignment. In recent years lattice structures composed of skyrmions have been discovered in certain bulk chiral magnets with non-centrosymmetric crystal structures. The magnetic phase diagrams of these materials share remarkable similarities despite great variations of the characteristic temperature, field, and length scales and regardless whether the underlying electronic state is that of a metal, semiconductor, or insulator., Comment: 38 pages, 8 figures

We report comprehensive small angle neutron scattering (SANS) 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 favours the phase for which a spatial modulation of the magnetization is closest to the pressure axis. Uniaxial pressures as low as 1kbar 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 how strain couples to magnetic order in the chiral magnet MnSi., Comment: 23 pages, includes supplement

We determined the bulk electronic structure in the prototypical Heusler compound Cu$_2$MnAl by measuring the Angular Correlation of Annihilation Radiation (2D-ACAR) using spin-polarized positrons. To this end, a new algorithm for reconstructing 3D densities from projections is introduced that allows us to corroborate the excellent agreement between our electronic structure calculations and the experimental data. The contribution of each individual Fermi surface sheet to the magnetization was identified, and summed to a total spin magnetic moment of $3.6\,\pm\,0.5\,\mu_B/\mathrm{f.u.}$.

A magnetic helix realizes a one-dimensional magnetic crystal with a period given by the pitch length $\lambda_h$. 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., Comment: 5 pages, 3 figures; (v2) slight modifications, published version

We report the low-temperature properties of $^{11}$B-enriched single-crystal CrB$_{2}$ as prepared from high-purity Cr and B powder by a solid-state reaction and optical float zoning. The electrical resistivity, $\rho_{\rm xx}$, Hall effect, $\rho_{\rm xy}$, and specific heat, $C$, are characteristic of an exchange-enhanced Fermi liquid ground state, which develops a slightly anisotropic spin gap $\Delta \approx 220\,{\rm K}$ below $T_{\rm N}=88\,{\rm K}$. This observation is corroborated by the absence of a Curie dependence in the magnetization for $T\to0$ reported in the literature. Comparison of $C$ with $d\rho_{\rm xx}/dT$, where we infer lattice contributions from measurements of VB$_2$, reveals strong antiferromagnetic spin fluctuations with a characteristic spin fluctuation temperature $T_{\rm sf}\approx 257\,{\rm K}$ in the paramagnetic state, followed by a pronounced second-order mean-field transition at $T_{\rm N}$, and unusual excitations around $\approx T_{\rm N}/2$. The pronounced anisotropy of $\rho_{\rm xx}$ above $T_{\rm N}$ is characteristic of an easy-plane anisotropy of the spin fluctuations consistent with the magnetization. The ratio of the Curie-Weiss to the N$\acute{\rm{e}}$el temperatures, $f=-\Theta_{\rm CW}/T_{\rm N}\approx 8.5$, inferred from the magnetization, implies strong geometric frustration. All physical properties are remarkably invariant under applied magnetic fields up to $14\,\,{\rm T}$, the highest field studied. In contrast to earlier suggestions of local-moment magnetism our study identifies CrB$_{2}$ as a weak itinerant antiferromagnet par excellence with strong geometric frustration., Comment: 15 pages, 9 figures

We report the development of a versatile module that permits fast and reliable use of focussing neutron guides under varying scattering angles. A simple procedure for setting up the module and neutron guides is illustrated by typical intensity patterns to highlight operational aspects as well as typical parasitic artefacts. Combining a high-precision alignment table with separate housings for the neutron guides on kinematic mounts, the change-over between neutron guides with different focussing characteristics requires no readjustments of the experimental set-up. Exploiting substantial gain factors, we demonstrate the performance of this versatile neutron scattering module in a study of the effects of uniaxial stress on the domain populations in the transverse spin density wave phase of single crystal Cr.

Heusler compounds exhibit a wide range of different electronic ground states and are hence expected to be applicable as functional materials in novel electronic and spintronic devices. Since the growth of large and defect-free Heusler crystals is still challenging, single crystals of Fe2TiSn and Cu2MnAl were grown by the optical floating zone technique. Two positron annihilation techniques -Angular Correlation of Annihilation Radiation (ACAR) and Doppler Broadening Spectroscopy (DBS)- were applied in order to study both, the electronic structure and lattice defects. Recently, we succeeded to observe clearly the anisotropy of the Fermi surface of Cu2MnAl, whereas the spectra of Fe2TiSn were disturbed by foreign phases. In order to estimate the defect concentration in different samples of Heusler compounds the positron diffusion length was determined by DBS using a monoenergetic positron beam.

Powder X-ray diffraction (PXRD) and single-crystal neutron scattering were used to study in detail the structural properties of the Cs2CuCl(4-x)Br(x) series, good realizations of layered triangular antiferromagnets. Detailed temperature-dependent PXRD reveal a pronounced anisotropy of the thermal expansion for the three different crystal directions of the orthorhombic structure without any structural phase transition down to 20 K. Remarkably, the anisotropy of the thermal expansion varies for different $x$, leading to distinct changes of the geometry of the local Cu environment as a function of temperature and composition. The refinement of the atomic positions confirms that for x=1 and 2, the Br atoms occupy distinct halogen sites in the [CuX4]-tetrahedra (X = Cl, Br). The precise structure data are used to calculate the magnetic exchange couplings using density functional methods for x=0. We observe a pronounced temperature dependence of the calculated magnetic exchange couplings, reflected in the strong sensitivity of the magnetic exchange couplings on structural details. These calculations are in good agreement with the experimentally established values for Cs2CuCl4 if one takes the low-temperature structure data as a starting point.

We report proof-of-principle measurements at the neutron resonance spin echo spectrometer RESEDA (MLZ) under large magnetic fields by means of Modulation of IntEnsity with Zero Effort (MIEZE). Our study demonstrates the feasibility of applying strong magnetic fields up to 17\,T at the sample while maintaining unchanged sub-$\mu$eV resolution. We find that the MIEZE-spin-echo resolution curve remains essentially unchanged as a function of magnetic field up to the highest fields available, promising access to high fields without need for additional fine-tuning of the instrument. This sets the stage for the experimental investigation of subtle field dependent phenomena, such as magnetic field-driven phase transitions in hard and soft condensed matter physics., Comment: 5 pages, 5 figures, conference QENS 2014 / WINS 2014

We report an experimental and computational study of the Hall effect in Mn$_{\rm 1-x}$Fe$_{\rm x}$Si, as complemented by measurements in Mn$_{\rm 1-x}$Co$_{\rm x}$Si, when helimagnetic order is suppressed under substitutional doping. For small $x$ the anomalous Hall effect (AHE) and the topological Hall effect (THE) change sign. Under larger doping the AHE remains small and consistent with the magnetization, while the THE grows by over a factor of ten. Both the sign and the magnitude of the AHE and the THE are in excellent agreement with calculations based on density functional theory. Our study provides the long-sought material-specific microscopic justification, that while the AHE is due to the reciprocal-space Berry curvature, the THE originates in real-space Berry phases., Comment: Phys. Rev. Lett., accepted for publication

Fermi liquid theory provides a remarkably powerful framework for the description of the conduction electrons in metals and their ordering phenomena, such as superconductivity, ferromagnetism, and spin- and charge-density-wave order. A different class of ordering phenomena of great interest concerns spin configurations that are topologically protected, that is, their topology can be destroyed only by forcing the average magnetization locally to zero. Examples of such configurations are hedgehogs (points at which all spins are either pointing inwards or outwards) or vortices. A central question concerns the nature of the metallic state in the presence of such topologically distinct spin textures. Here we report a high-pressure study of the metallic state at the border of the skyrmion lattice in MnSi, which represents a new form of magnetic order composed of topologically non-trivial vortices. When long-range magnetic order is suppressed under pressure, the key characteristic of the skyrmion lattice - that is, the topological Hall signal due to the emergent magnetic flux associated with their topological winding - is unaffected in sign or magnitude and becomes an important characteristic of the metallic state. The regime of the topological Hall signal in temperature, pressure and magnetic field coincides thereby with the exceptionally extended regime of a pronounced non-Fermi-liquid resistivity. The observation of this topological Hall signal in the regime of the NFL resistivity suggests empirically that spin correlations with non-trivial topological character may drive a breakdown of Fermi liquid theory in pure metals.

We report detailed low temperature magnetotransport and magnetization measurements in MnSi under pressures up to $\sim12\,{\rm kbar}$. Tracking the role of sample quality, pressure transmitter, and field and temperature history allows us to link the emergence of a giant topological Hall resistivity $\sim50\,{\rm n\Omega cm}$ to the skyrmion lattice phase at ambient pressure. We show that the remarkably large size of the topological Hall resistivity in the zero-temperature limit must be generic. We discuss various mechanisms which can lead to the much smaller signal at elevated temperatures observed at ambient pressure.

We report on state-of-the-art scanning probe microscopy measurements performed in a pulse tube based top-loading closed-cycle cryostat with a base temperature of 4 K and a 9 T magnet. We decoupled the sample space from the mechanical and acoustic noise from the cryocooling system to enable scanning probe experiments. The extremely low vibration amplitudes in our system enabled successful imaging of 0.39 nm lattice steps on single crystalline SrTiO$_{3}$ as well as magnetic vortices in Bi$_{2}$Sr$_{2}$CaCu$_{2}$O$_{8+x}$ superconductor. Fine control over sample temperature and applied magnetic field further enabled us to probe the helimagnetic and the skyrmion-lattice phases in Fe$_{0.5}$Co$_{0.5}$Si with unprecedented signal-to-noise ratio of 20:1. Finally, we demonstrate for the first time quartz-crystal tuning fork shear-force microscopy in a closed-cycle cryostat.

We report spherical neutron polarimetry (SNP) and discuss the spin-flip scattering cross sections as well as the chiral fraction $\eta$ close to the helimagnetic transition in MnSi. For our study, we have developed a miniaturised SNP device that allows fast data collection when used in small angle scattering geometry with an area detector. Critical spin-flip scattering is found to be governed by chiral paramagnons that soften on a sphere in momentum space. Carefully accounting for the incoherent spin-flip background, we find that the resulting chiral fraction $\eta$ decreases gradually above the helimagnetic transition reflecting a strongly renormalised chiral correlation length with a temperature dependence in excellent quantitative agreement with the Brazovskii theory for a fluctuation-induced first order transition., Comment: 5 pages, 3 figures