The lack of inversion symmetry in the crystal lattice of magnetic materials gives rise to complex noncollinear spin orders through interactions of a relativistic nature, resulting in interesting physical phenomena, such as emergent electromagnetism. Studies of cubic chiral magnets revealed a universal magnetic phase diagram composed of helical spiral, conical spiral, and skyrmion crystal phases. We report a remarkable deviation from this universal behavior. By combining neutron diffraction with magnetization measurements, we observe a new multidomain state in Cu₂OSeO₃. Just below the upper critical field at which the conical spiral state disappears, the spiral wave vector rotates away from the magnetic field direction. This transition gives rise to large magnetic fluctuations. We clarify the physical origin of the new state and discuss its multiferroic properties.

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The research presented in this thesis focuses on chiral magnets, where skyrmion lattices are stablised by magnetic fields. Neutron scattering, magnetisation and magnetic susceptibility measurements have been performed on several typical chiral magnets such as the multiferroic insulator Cu2OSeO3 and the metallic MnSi and FeGe...@en

We present a comprehensive Small Angle Neutron Scattering (SANS) and Neutron Spin Echo Spectroscopy (NSE) study of the structural and dynamical aspects of the helimagnetic transition in Fe_1-xCo_xSi with x = 0.30. In contrast to the sharp transition observed in the archetype chiral magnet MnSi, the transition in Fe_1-xCo_xSi is gradual and long-range helimagnetic ordering coexists with short-range correlations over a wide temperature range. The dynamics are more complex than in MnSi and involve long relaxation times with a stretched exponential relaxation which persists even under magnetic field. These results in conjunction with an analysis of the hierarchy of the relevant length scales show that the helimagnetic transition in Fe_1-xCo_xSi differs substantially from the transition in MnSi and question the validity of a universal approach to the helimagnetic transition in chiral magnets.@en

Magnetic skyrmions are nanosized topologically protected spin textures with particlelike 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 Cu2OSeO3 and the archetype chiral magnet MnSi. The results reveal that the orientation of the skyrmion lattice is primarily determined by the magnetic field direction with respect to the crystallographic lattice. In addition, it is also influenced by the magnetic history of the sample, which can induce metastable lattices. Kinetic measurements show that these metastable skyrmion lattices may or may not relax to their equilibrium positions under macroscopic relaxation times. Furthermore, multidomain lattices may form when two or more equivalent crystallographic directions are favored by spin-orbit coupling and oriented perpendicular to the magnetic field.@en

The reference chiral helimagnet MnSi is the first system where Skyrmion lattice correlations have been reported. At a zero magnetic field the transition at TC to the helimagnetic state is of first order. Above TC, in a region dominated by precursor phenomena, neutron scattering shows the buildup of strong chiral fluctuating correlations over the surface of a sphere with radius 2π/, where is the pitch of the helix. It has been suggested that these fluctuating correlations drive the helical transition to first order following a scenario proposed by Brazovskii for liquid crystals. We present a comprehensive neutron scattering study under magnetic fields, which provides evidence that this is not the case. The sharp first order transition persists for magnetic fields up to 0.4 T whereas the fluctuating correlations weaken and start to concentrate along the field direction already above 0.2 T. Our results thus disconnect the first order nature of the transition from the precursor fluctuating correlations. They also show no indication for a tricritical point, where the first order transition crosses over to second order with increasing magnetic field. In this light, the nature of the first order helical transition and the precursor phenomena above TC, both of general relevance to chiral magnetism, remain an open question.

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Small angle neutron scattering measurements on a bulk single crystal of the doped chiral magnet Fe1-xCoxSi with x=0.3 reveal a pronounced effect of the magnetic history and cooling rates on the magnetic phase diagram. The extracted phase diagrams are qualitatively different for zero and field cooling and reveal a metastable skyrmion lattice phase outside the A phase for the latter case. These thermodynamically metastable skyrmion lattice correlations coexist with the conical phase and can be enhanced by increasing the cooling rate. They appear in a wide region of the phase diagram at temperatures below the A phase but also at fields considerably smaller or higher than the fields required to stabilize the A phase.

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The spatial and temporal correlations of magnetic moments in the paramagnetic regime of (Mn,Fe)2(P,Si) have been investigated by means of polarized neutron diffraction and muon-spin relaxation techniques. Short-range magnetic correlations are present at temperatures far above the ferromagnetic transition temperature (TC). This leads to deviations of paramagnetic susceptibility from Curie-Weiss behavior. These short-range magnetic correlations extend in space, slow down with decreasing temperature, and finally develop into long-range magnetic order at TC.

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We present an investigation of the magnetic-field-temperature phase diagram of Cu2OSeO3 based on dc magnetization 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 Tc=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 nonexponential. Consequently the borders between the different phases depend on the specific criteria and frequency used and an unambiguous determination is not possible.

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