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Register a new userNew magnetic phase of the chiral skyrmion material Cu2OSeO3
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The lack of inversion symmetry in the crystal lattice of magnetic materials gives rise to complex non-collinear spin orders through interactions of 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. Here, we report a remarkable deviation from this universal behavior. By combining neutron diffraction with magnetization measurements we observe a new multi-domain 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 physical origin of the new state and discuss its multiferroic properties.
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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 $(0bar{1}1)$ 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 a region of the field-temperature phase diagram that is consistent with previous reports. Our measurements show that not only the field-polarised phase but also the helical ground state are made up of ferrimagnetic clusters instead of individual spins. These clusters are distorted Cu tetrahedra, where the spin on one Cu ion is anti-aligned with the spin on the three other Cu ions.
In the cubic chiral magnet Cu2OSeO3 a low-temperature skyrmion state (LTS) and a concomitant tilted conical state are observed for magnetic fields parallel to <100>. In this work, we report on the dynamic resonances of these novel magnetic states. After promoting the nucleation of the LTS by means of field cycling, we apply broadband microwave spectroscopy in two experimental geometries that provide either predominantly in-plane or out-of-plane excitation. By comparing the results to linear spin-wave theory, we clearly identify resonant modes associated with the tilted conical state, the gyrational and breathing modes associated with the LTS, as well as the hybridization of the breathing mode with a dark octupole gyration mode mediated by the magnetocrystalline anisotropies. Most intriguingly, our findings suggest that under decreasing fields the hexagonal skyrmion lattice becomes unstable with respect to an oblique deformation, reflected in the formation of elongated skyrmions.
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 $q parallel <001>$ upon approaching $T_c$. Near the phase boundary between these two states, the external magnetic field induces a 30$^circ$-rotation of the skyrmion lattice. This suggests a delicate balance between the magnetic anisotropy and the spin texture near $T_c$, such that even a small perturbation significantly affects the ordering pattern of the skyrmions.
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. The new skyrmion phase is thermodynamically disconnected from the well-known, nearly-isotropic, high-temperature phase, and exists, in contrast, when the external magnetic field is oriented along the $langle100rangle$ crystal axis only. Theoretical modelling provides evidence that the stabilization mechanism is given by well-known cubic anisotropy terms, and accounts for an additional observation of metastable helices tilted away from the applied field. The identification of two distinct skyrmion phases in the same material and the generic character of the underlying mechanism suggest a new avenue for the discovery, design, and manipulation of topological spin textures.
Polar lacunar spinels, such as GaV$_4$S$_8$ and GaV$_4$Se$_8$, were proposed to host skyrmion phases under magnetic field. In this work, we put forward, as a candidate for Neel-type skyrmion lattice, the isostructural GaMo$_4$S$_8$, here systematically studied via both first-principles calculations and Monte Carlo simulations of model Hamiltonian. Electric polarization, driven by Jahn-Teller distortion, is predicted to arise in GaMo$_4$S$_8$, showing a comparable size but an opposite sign with respect to that evaluated in V-based counterparts and explained in terms of different electron counting arguments and resulting distortions. Interestingly, a larger spin-orbit coupling of 4d orbitals with respect to 3d orbitals in vanadium-spinels leads to stronger Dzyaloshinskii-Moriya interactions, which are beneficial to stabilize a cycloidal spin texture, as well as smaller-sized skyrmions (radius<10 nm). Furthermore, the possibly large exchange anisotropy of GaMo4S8 may lead to a ferroelectric-ferromagnetic ground state, as an alternative to the ferroelectric-skyrmionic one, calling for further experimental verification.
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