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Register a new userEstablishing the fundamental magnetic interactions in the chiral skyrmionic Mott insulator Cu2OSeO3 by terahertz electron spin resonance
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The recent discovery of skyrmions in Cu$_2$OSeO$_3$ has established a new platform to create and manipulate skyrmionic spin textures. We use high-field electron spin resonance (ESR) spectroscopy combining a terahertz free electron laser and pulsed magnetic fields up to 64 T to probe and quantify its microscopic spin-spin interactions. Besides providing direct access to the long-wavelength Goldstone mode, this technique probes also the high-energy part of the excitation spectrum which is inaccessible by standard low-frequency ESR. Fitting the behavior of the observed modes in magnetic field to a theoretical framework establishes experimentally that the fundamental magnetic building blocks of this skyrmionic magnet are rigid, highly entangled and weakly coupled tetrahedra.
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Dielectric properties were investigated under various magnitudes and directions of magnetic field (H) for a chiral magnetic insulator Cu2OSeO3. We found that the skyrmion crystal induces electric polarization (P) along either in-plane or out-of-plane direction of the spin vortices depending on the applied H-direction. The observed H-dependence of P in ferrimagnetic, helimagnetic, and skyrmion crystal state can be consistently described by the d-p hybridization model, highlighting an important role of relativistic spin-orbit interaction in the magnetoelectric coupling in Cu2OSeO3. Our analysis suggests that each skyrmion particle can locally carry electric dipole or quadrupole, which implies that the dynamics of skyrmions are controllable by the external electric field.
The magneto-electric (ME) coupling on spin-wave resonances in single-crystal Cu2OSeO3 was studied by a novel technique using electron spin resonance combined with electric field modulation. An external electric field E induces a magnetic field component mu_0 H^i = gamma E along the applied magnetic field H with gamma=0.7(1) mu T/(V/mm) at 10 K. We found that ME coupling strength gamma is temperature dependent and highly anisotropic. gamma(T) nearly follows that of spin susceptibility J(T) and rapidly decreases above the Curie temperature Tc. The ratio gamma/J monotonically decreases with increasing temperature without an anomaly at Tc.
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.
We show that continuous and spin-lattice models of chiral ferro- and antiferromagnets provide the existence of an infinite number of stable soliton solutions of any integer topological charge. A detailed description of the morphology of new skyrmions and the corresponding energy dependencies are provided. The considered model is general, and is expected to predict a plethora of particle-like states which may occur in various chiral magnets including atomic layers, e.g., PdFe/Ir(111), rhombohedral GaV$_4$S$_8$ semiconductor, B20-type alloys as Mn$_{1-x}$Fe$_x$Ge, Mn$_{1-x}$Fe$_x$Si, Fe$_{1-x}$Co$_x$Si, Cu$_2$OSeO$_3$, acentric tetragonal Heusler compounds.
In this work, we present a comprehensive study of the low energy optical magnetic response of the skyrmionic Mott insulator Cu$_2$OSeO$_3$ via high resolution time-domain THz spectroscopy. In zero field, a new magnetic excitation not predicted by spin-wave theory with frequency $f$ = 2.03 THz is observed and shown, with accompanying time-of-flight neutron scattering experiments, to be a zone folded magnon from the $mathrm{R}$ to $mathrm{Gamma}$ points of the Brillouin zone. Highly sensitive polarimetry experiments performed in weak magnetic fields, $mu_0$H $<$ 200 mT, observe Faraday and Kerr rotations which are proportional to the sample magnetization, allowing for optical detection of the skyrmion phase and construction of a magnetic phase diagram. From these measurements, we extract a critical exponent of $beta$ = 0.35 $pm$ 0.04, in good agreement with the expected value for the 3D Heisenberg universality class of $beta$ = 0.367. In large magnetic fields, $mu_0$H $>$ 5 T, we observe the magnetically active uniform mode of the ferrimagnetic field polarized phase whose dynamics as a function of field and temperature are studied. In addition to extracting a $g_text{eff}$ = 2.08 $pm$ 0.03, we observe the uniform mode to decay through a non-Gilbert damping mechanism and to possesses a finite spontaneous decay rate, $Gamma_0$ $approx$ 25 GHz, in the zero temperature limit. Our observations are attributed to Dzyaloshinkii-Moriya interactions, which have been proposed to be exceptionally strong in Cu$_2$OSeO$_3$ and are expected to impact the low energy magnetic response of such chiral magnets.
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