The growth of single crystals of FeCl₃, through sublimation and from the melt, is presented alongside a thorough investigation of their magnetostructural properties through a combination of DC magnetization and AC magnetic susceptibility measurements, single crystal X-ray diffraction (SCXRD), neutron powder diffraction (NPD) and small-angle neutron scattering (SANS). A new chiral polymorph of FeCl₃ is identified, crystallizing in the non-centrosymmetric space group P3₁. NPD and SANS reveal that a weakly first-order magnetic phase transition occurs from a paramagnetic phase with significant short-range correlations to an antiferromagnetic phase at T_N = 8.6 K, best described by the magnetic propagation vector k = (1/2, 0, 1/3) which differs from the previously reported magnetic structure of the well-known centrosymmetric polymorph (space group R3̄). We show that disordered crystallographic models including a large number of stacking faults are required to accurately reproduce the scattering observed in NPD patterns, preventing full determination of the magnetic structure. The magnetic field and temperature-dependent behavior of the intensities of the k = (1/2, 0, 2/3) and (1/2, 0, 5/3) magnetic Bragg peaks measured by SANS suggest that a field-induced spin reorientation occurs at H = 40 kOe when H‖c-axis and at a significantly lower field of H ≈ 25 kOe when H⊥c-axis. Above these magnetic fields in both cases the spins lie predominantly in the basal plane. The long-range magnetic ordering and the field-induced transitions observed in the neutron scattering experiments coincide with anomalies observed in the magnetisation versus both temperature and applied field along the principal crystal directions.

We present a systematic study of tilted spiral states obtained theoretically within the classical Dzyaloshinskii model for magnetic states in cubic non-centrosymmetric ferromagnets. Such tilted spirals are shown to stabilize under the competing effect of cubic and exchange anisotropies inherent to cubic helimagnets. By focusing on the internal structure of these spirals and their field-driven behaviour for different aspect ratios of the anisotropy coefficients, we are able to capture the main features of the experimental findings in a bulk cubic helimagnet Cu₂OSeO₃ and to make a step further towards a complete quantitative model of this chiral magnet. In particular, we show that for strong anisotropy values (which experimentally correspond to low temperatures near zero) there exist an angular separation between the conical and tilted spirals, i.e., the conical spiral flips into a tilted state and immediately composes some finite angle with respect to the field direction. As the anisotropy ratio decreases, such a transition between two spiral states becomes almost continuous and corresponds to higher temperatures at the experiments. In addition, we investigate the field-driven reorientation of metastable skyrmion lattices induced by the competing anisotropies, which may be responsible for some peculiarities at the experimental phase diagrams of Cu₂OSeO₃.

The bulk helimagnet Cu2OSeO3 represents a unique example in the family of B20 cubic helimagnets exhibiting a tilted spiral and skyrmion phase at low temperatures when the magnetic field is applied along the easy (001) crystallographic direction. Here we present a systematic study of the stability and ordering of these low-temperature magnetic states. We focus our attention on the temperature and field dependencies of the tilted spiral state that we observe persisting up to above T=35 K, i.e., up to higher temperatures than reported so far. We discuss these results in the frame of the phenomenological theory introduced by Dzyaloshinskii in an attempt to reach a quantitative description of the experimental findings. We find that the anisotropy constants, which are the drivers behind the observed behavior, exhibit a pronounced temperature dependence. This explains the differences in the behavior observed at high temperatures (above T=18 K), where the cubic anisotropy is weak, and at low temperatures (below T=18 K), where a strong cubic anisotropy induces an abrupt appearance of the tilted spirals out of the conical state and enhances the stability of skyrmions.

Cu2OSeO3 represents a unique example in the family of B20 cubic helimagnets with a tilted spiral and a low-temperature skyrmion phase arising for magnetic fields applied along the easy crystallographic (100) axes. Although the stabilization mechanism of these phases can be accounted for by cubic magnetic anisotropy, the skyrmion nucleation process is still an open question, since the stability region of the skyrmion phase displays strongly hysteretic behavior with different phase boundaries for increasing and decreasing magnetic fields. Here, we address this important point using micromagnetic simulations and come to the conclusion that skyrmion nucleation is underpinned by the reorientation of spiral domains occurring near the critical magnetic fields of the phase diagrams: HC1, the critical field of the transition between the helical and conical/tiled spiral phase, and HC2, the critical field between the conical/tiled spiral and the homogenous phase. By studying a wide variety of cases we show that domain walls may have a 3D structure. Moreover, they can carry a finite topological charge stemming from half-skyrmions (merons) also permitting along-the-field and perpendicular-to-the-field orientation. Thus, domain walls may be envisioned as nucleation source of skyrmions that can form thermodynamically stable and metastable lattices as well as skyrmion networks with misaligned skyrmion tubes. The results of numerical simulations are discussed in view of recent experimental data on chiral magnets, in particular, for the bulk cubic helimagnet Cu2OSeO3.

We present a comprehensive investigation of the magnetic properties of stage-1 graphite intercalated FeCl3 using a combination of DC and AC magnetic susceptibility, thermoremanent magnetization, and field-dependent magnetization measurements. This van der Waals system, with a centrosymmetric honeycomb lattice, combines frustration and disorder, due to intercalation, and may be hosting topologically nontrivial magnetic phases. Our study identifies two magnetic phase transitions at Tf1≈4.2 K and at Tf2≈2.7 K. We find that the paramagnetic state, for T>Tf1, is dominated by short-range ferromagnetic correlations. These build up well above Tf1 and lead to a significant change in magnetic entropy, which reaches ΔSMPk=-5.52 J kg-1K-1 at 7 T. Between Tf1 and Tf2, we observe slow spin dynamics characteristic of a cluster glasslike state, whereas for T<Tf2, our results indicate the onset of a low-temperature long-range ordered state. The analysis of the experimental results leads to a complex phase diagram, which may serve as a reference for future investigations searching for topological nontrivial phases in this system.

In-situ Neutron Diffraction and Small-Angle Neutron Scattering (SANS) are employed for the first time simultaneously in order to reveal the interaction between the austenite to ferrite phase transformation and the precipitation kinetics during isothermal annealing at 650 and at 700 °C in three steels with different vanadium (V) and carbon (C) concentrations. Austenite-to-ferrite phase transformation is observed in all three steels at both temperatures. The phase transformation is completed during a 10 h annealing treatment in all cases. The phase transformation is faster at 650 than at 700 °C for all alloys. Additions of vanadium and carbon to the steel composition cause a retardation of the phase transformation. The effect of each element is explained through its contribution to the Gibbs free energy dissipation. The austenite-to-ferrite phase transformation is found to initiate the vanadium carbide precipitation. Larger and fewer precipitates are detected at 700 than at 650 °C in all three steels, and a larger number density of precipitates is detected in the steel with higher concentrations of vanadium and carbon. After 10 h of annealing, the precipitated phase does not reach the equilibrium fraction as calculated by ThermoCalc. The external magnetic field applied during the experiments, necessary for the SANS measurements, causes a delay in the onset and time evolution of the austenite-to-ferrite phase transformation and consequently on the precipitation kinetics.

We study the evolution of the low-temperature field-induced magnetic defects observed under an applied magnetic field in a series of frustrated amorphous ferromagnets (Fe_1-xMn_x)₇₅P₁₆B₃Al₃ (“a-Fe_1-xMn_x”). Combining small-angle neutron scattering and Monte Carlo simulations, we show that the morphology of these defects resemble that of quasi-bidimensional spin vortices. They are observed in the so-called “reentrant” spin-glass (RSG) phase, up to the critical concentration x_C≈ 0.36 which separates the RSG and “true” spin glass (SG) within the low temperature part of the magnetic phase diagram of a-Fe_1−xMn_x. These textures systematically decrease in size with increasing magnetic field or decreasing the average exchange interaction, and they finally disappear in the SG sample (x= 0.41), being replaced by field-induced correlations over finite length scales. We argue that the study of these nanoscopic defects could be used to probe the critical line between the RSG and SG phases.

SESANS data analysis has been implemented in the SasView software package, allowing SESANS experiments to be analyzed using a numerical Hankel transformation of isotropic small-angle scattering (SAS) models. The error of the numerical approximation is three orders of magnitude below typical experimental errors. All advanced data fitting features of SasView (multi-model fitting, batch fitting, and simultaneous/constrained fitting) are now also available for SESANS and this is demonstrated by examples of fitting SAS models to SESANS measurements.

Neutron Spin Echo methods (NSE) use Larmor labelling to measure the precession phase of the neutron beam polarization around well-defined magnetic fields. Scattering by a sample can affect the resulting precession phase providing information on the sample's structure and dynamics with high accuracy and resolution. A major limitation for the performance of Neutron Spin Echo instruments is the homogeneity of the precession magnetic fields. Here we investigate the influence of the new 'pancake' moderator, which is being built at the European Spallation Source, on the design of a Neutron Spin Echo spectrometer. The calculations show clear gains when the height to width ratios of the rectangular beam cross-sections mimic those of the ESS 'pancake' moderator beams. In such a case the homogeneity of the magnetic field integrals could improve by at least 30%. However, the calculations show that will not be possible to preserve a high resolution and at the same time reduce the length of the instrument. Consequently, NSE spectrometers will perform better at the ESS but they will not be substantially compacter than at other neutron sources e.g. ILL or FRM2.

In-situ Small-Angle Neutron Scattering (SANS) is used to determine the time evolution of the chemical composition of precipitates at 650 °C and 700 °C in three micro-alloyed steels with different vanadium (V) and carbon (C) concentrations. Precipitates with a distribution of substoichiometric carbon-to-metal ratios are measured in all steels. The precipitates are initially metastable with a high iron (Fe) content, which is gradually being substituted by vanadium during isothermal annealing. Eventually a plateau in the composition of the precipitate phase is reached. Faster changes in the precipitate chemical composition are observed at the higher temperature in all steels because of the faster vanadium diffusion at 700 °C. At both temperatures, the addition of more vanadium and more carbon to the steel has an accelerating effect on the evolution of the precipitate composition as a result of a higher driving force for precipitation. Addition of vanadium to the nominal composition of the steel leads to more vanadium rich precipitates, with less iron and a smaller carbon-to-metal ratio. Atom Probe Tomography (APT) shows the presence of precipitates with a distribution of carbon-to-metal ratios, ranging from 0.75 to 1, after 10 h of annealing at 650 °C or 700 °C in all steels. These experimental results are coupled to ThermoCalc equilibrium calculations and literature findings to support the Small-Angle Neutron Scattering results.

Interphase precipitation occurring during solid-state phase transformations in micro-alloyed steels is generally studied through transmission electron microscopy, atom probe tomography, and ex situ measurements of Small-Angle Neutron Scattering (SANS). The advantage of SANS over the other two characterization techniques is that SANS allows for the quantitative determination of size distribution, volume fraction, and number density of a statistically significant number of precipitates within the resulting matrix at room temperature. However, the performance of ex situ SANS measurements alone does not provide information regarding the probable correlation between interphase precipitation and phase transformations. This limitation makes it necessary to perform in situ and simultaneous studies on precipitation and phase transformations in order to gain an in-depth understanding of the nucleation and growth of precipitates in relation to the evolution of austenite decomposition at high temperatures. A furnace is, thus, designed and developed for such in situ studies in which SANS measurements can be simultaneously performed with neutron diffraction measurements during the application of high-temperature thermal treatments. The furnace is capable of carrying out thermal treatments involving fast heating and cooling as well as high operation temperatures (up to 1200 °C) for a long period of time with accurate temperature control in a protective atmosphere and in a magnetic field of up to 1.5 T. The characteristics of this furnace give the possibility of developing new research studies for better insight of the relationship between phase transformations and precipitation kinetics in steels and also in other types of materials containing nano-scale microstructural features.

The archetype cubic chiral magnet MnSi is home to some of the most fascinating states in condensed matter, such as skyrmions and a non-Fermi-liquid behavior in conjunction with a topological Hall effect under hydrostatic pressure. Using small angle neutron scattering, we study the evolution of the helimagnetic, conical, and skyrmionic correlations with increasing hydrostatic pressure. We show that the helical propagation vector smoothly reorients from (111) to (100) at intermediate pressures. At higher pressures, above the critical pressure, the long-range helimagnetic order disappears at zero magnetic field. Nevertheless, skyrmion lattices and conical spirals form under magnetic fields, in a part of the phase diagram where a topological Hall effect and a non-Fermi-liquid behavior have been reported. These unexpected results shed light on the puzzling behavior of MnSi at high pressures and the mechanisms that destabilize the helimagnetic long-range order at the critical pressure.