Establishing the fundamental magnetic interactions in the chiral skyrmionic Mott insulator Cu2OSeO3 by terahertz electron spin resonance

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.Comment: 5 pages, 3 Figure

Spin excitations in the skymion host Cu2OSeO3

We have used inelastic neutron scattering to measure the magnetic excitation spectrum along the high-symmetry directions of the first Brillouin zone of the magnetic skyrmion hosting compound Cu$_2$OSeO$_3$. The majority of our scattering data are consistent with the expectations of a recently proposed model for the magnetic excitations in Cu$_2$OSeO$_3$, and we report best-fit parameters for the dominant exchange interactions. Important differences exist, however, between our experimental findings and the model expectations. These include the identification of two energy scales that likely arise due to neglected anisotropic interactions. This feature of our work suggests that anisotropy should be considered in future theoretical work aimed at the full microscopic understanding of the emergence of the skyrmion state in this material.Comment: 5 pages, 6 figure

Spin-stretching modes in anisotropic magnets: spin-wave excitations in the multiferroic Ba2CoGe2O7

We studied spin excitations of the multiferroic Ba2CoGe2O7 in high magnetic fields up to 33 T. In the electron spin resonance and far infrared absorption spectra we found several spin excitations beyond the two conventional magnon modes expected for such a two-sublattice antiferromagnet. We show that a multi-boson spin-wave theory can capture these unconventional modes, that include spin-stretching modes associated with an oscillating magnetic dipole (or only quadrupole) moment. The lack of the inversion symmetry allows these modes to become electric dipole active. We expect that the spin-stretching modes can be generally observed in inelastic neutron scattering and light absorption experiments in a broad class of ordered S > 1/2 spin systems with strong single-ion anisotropy and/or non-centrosymmetric lattice structure.Comment: 5+4 pages, 3 figures, supplement added, manuscript revise

In-situ electric field control of THz non-reciprocal directional dichroism in the multiferroic Ba2_2CoGe2_2O7_7

Non-reciprocal directional dichroism, also called the optical-diode effect, is an appealing functional property inherent to the large class of non-centrosymmetric magnets. However, the in-situ electric control of this phenomenon is challenging as it requires a set of conditions to be fulfilled: Special symmetries of the magnetic ground state, spin-excitations with comparable magnetic- and electric-dipole activity and switchable electric polarization. We demonstrate the isothermal electric switch between domains of Ba$_2$CoGe$_2$O$_7$ possessing opposite magnetoelectric susceptibilities. Combining THz spectroscopy and multiboson spin-wave analysis, we show that unbalancing the population of antiferromagnetic domains generates the non-reciprocal light absorption of spin excitations.Comment: version accepte

Magnon spectrum of the helimagnetic insulator Cu2OSeO3

Complex low-temperature-ordered states in chiral magnets are typically governed by a competition between multiple magnetic interactions. The chiral-lattice multiferroic Cu2OSeO3 became the first insulating helimagnetic material in which a long-range order of topologically stable spin vortices known as skyrmions was established. Here we employ state-of-the-art inelastic neutron scattering to comprehend the full three-dimensional spin-excitation spectrum of Cu2OSeO3 over a broad range of energies. Distinct types of high- and low-energy dispersive magnon modes separated by an extensive energy gap are observed in excellent agreement with the previously suggested microscopic theory based on a model of entangled Cu4 tetrahedra. The comparison of our neutron spectroscopy data with model spin-dynamical calculations based on these theoretical proposals enables an accurate quantitative verification of the fundamental magnetic interactions in Cu2OSeO3 that are essential for understanding its abundant low-temperature magnetically ordered phases