We report a long-wavelength helimagnetic superstructure in bulk samples of the ferrimagnetic insulator Cu2OSeO3. The magnetic phase diagram associated with the helimagnetic modulation inferred from small-angle neutron scattering and magnetization measurements includes a skyrmion lattice phase and is strongly reminiscent of MnSi, FeGe, and Fe(1-x)Co(x)Si, i.e., binary isostructural siblings of Cu2OSeO3 that order helimagnetically. The temperature dependence of the specific heat of Cu2OSeO3 is characteristic of nearly critical spin fluctuations at the helimagnetic transition. This provides putative evidence for effective spin currents as the origin of enhancements of the magnetodielectric response instead of atomic displacements considered so far.

An overview of one-and two-dimensional quantum spin systems based on transition-metal oxides and halides of current interest is given, such as spinPeierls, spin-dimer, geometrically frustrated and ladder systems. The most significant and outstanding contributions of magnetic light scattering to the understanding of these materials are discussed and compared to results of other spectroscopies and thermodynamic measurements.

Raman scattering has been employed to investigate lattice and magnetic excitations of the honeycomb Kitaev material α-RuCl3 and its Heisenberg counterpart CrCl3. Our phonon Raman spectra give evidence for a first-order structural transition from a monoclinic to a rhombohedral structure for both compounds. Significantly, only α-RuCl3 features a large thermal hysteresis, consistent with the formation of a wide phase of coexistence. In the related temperature interval of 70 − 170 K, we observe a hysteretic behavior of magnetic excitations as well. The stronger magnetic response in the rhombohedral compared to the monoclinic phase evidences a coupling between the crystallographic structure and low-energy magnetic response. Our results demonstrate that the Kitaev magnetism concomitant with fractionalized excitations is susceptible to small variations of bonding geometry.

Susceptibility, specific heat, and muon spin rotation measurements on high-quality single crystals of Na 0.82 CoO 2 have revealed bulk antiferromagnetism with Néel temperature T N ϭ19.8Ϯ0.1 K and an ordered moment perpendicular to the CoO 2 layers. The magnetic order encompasses nearly 100% of the crystal volume. The susceptibility exhibits a broad peak around 30 K, characteristic of two-dimensional antiferromagnetic fluctuations. The in-plane resistivity is metallic at high temperatures and exhibits a minimum at T N .

The fractionalization of elementary excitations in quantum spin systems is a central theme in current condensed matter physics. The Kitaev honeycomb spin model provides a prominent example of exotic fractionalized quasiparticles, composed of itinerant Majorana fermions and gapped gauge fluxes. However, identification of the Majorana fermions in a three-dimensional honeycomb lattice remains elusive. Here we report spectroscopic signatures of fractional excitations in the harmonic-honeycomb iridates β- and γ-Li2IrO3. Using polarization-resolved Raman spectroscopy, we find that the dynamical Raman response of β- and γ-Li2IrO3 features a broad scattering continuum with distinct polarization and composition dependence. The temperature dependence of the Raman spectral weight is dominated by the thermal damping of fermionic excitations. These results suggest the emergence of Majorana fermions from spin fractionalization in a three-dimensional Kitaev–Heisenberg system.