Berezinskii-Kosterlitz-Thouless Type Scenario in Molecular Spin Liquid AACr2_2O4_4

The spin relaxation in chromium spinel oxides $A$Cr$_{2}$O$_{4}$ ($A=$ Mg, Zn, Cd) is investigated in the paramagnetic regime by electron spin resonance (ESR). The temperature dependence of the ESR linewidth indicates an unconventional spin-relaxation behavior, similar to spin-spin relaxation in the two-dimensional (2D) chromium-oxide triangular lattice antiferromagnets. The data can be described in terms of a generalized Berezinskii-Kosterlitz-Thouless (BKT) type scenario for 2D systems with additional internal symmetries. Based on the characteristic exponents obtained from the evaluation of the ESR linewidth, short-range order with a hidden internal symmetry is suggested.Comment: 7 pages, 4 figure

On the complexity of spinels: magnetic, electronic, and polar ground states

This review summarizes more than 100 years of research on spinel compounds, mainly focusing on the progress in understanding their magnetic, electronic, and polar properties during the last two decades. Many spinel compounds are magnetic insulators or semiconductors; however, a number of spinel-type metals exists including superconductors and some rare examples of d-derived heavy-fermion compounds. In the early days, they gained importance as ferrimagnetic or even ferromagnetic insulators with relatively high saturation magnetization and high ordering temperatures, with magnetite being the first magnetic mineral known to mankind. However, spinels played an outstanding role in the development of concepts of magnetism, in testing and verifying the fundamentals of magnetic exchange, in understanding orbital-ordering and charge-ordering phenomena. In addition, the A- site as well as the B-site cations in the spinel structure form lattices prone to strong frustration effects resulting in exotic ground-state properties. In case the A-site cation is Jahn-Teller active, additional entanglements of spin and orbital degrees of freedom appear, which can give rise to a spin-orbital liquid or an orbital glass state. The B-site cations form a pyrochlore lattice, one of the strongest contenders of frustration in three dimensions. In addition, in spinels with both cation lattices carrying magnetic moments, competing magnetic exchange interactions become important, yielding ground states like the time-honoured triangular Yafet-Kittel structure. Finally, yet importantly, there exists a long-standing dispute about the possibility of a polar ground state in spinels, despite their reported overall cubic symmetry. Indeed, over the years number of multiferroic spinels were identified.Comment: 118 pages, 60 figure

Spin dynamics of the ordered phase of the frustrated antiferromagnet ZnCr2O4: a magnetic resonance study

We present an elaborate electron-spin resonance study of the low-energy dynamics and magnetization in the ordered phase of the frustrated spinel ZnCr2O4. We observe several resonance modes corresponding to different structural domains and found that the number of domains can be easily reduced by field-cooling the sample through the transition point. To describe the observed antiferromagnetic resonance spectra it is necessary to take into account an orthorhombic lattice distortion in addition to the earlier reported tetragonal distortion which both appear at the antiferromagnetic phase transition

Orbital Freezing in FeCr2S4 Studied by Dielectric Spectroscopy

Broadband dielectric spectroscopy has been performed on single-crystalline FeCr2S4 revealing a transition into a low-temperature orbital glass phase and on polycrystalline FeCr2S4 where long-range orbital order is established via a cooperative Jahn-Teller transition. The freezing of the orbital moments is revealed by a clear relaxational behavior of the dielectric permittivity, which allows a unique characterization of the orbital glass transition. The orbital relaxation dynamics continuously slows down over six decades in time, before at the lowest temperatures the glass transition becomes suppressed by quantum tunneling.Comment: 4 pages, 4 figure

Magnetic Excitations in the Multiferroic N\'eel-type Skyrmion Host GaV4_4S8_8

Broadband microwave spectroscopy has been performed on single-crystalline GaV$_4$S$_8$, which exhibits a complex magnetic phase diagram including cycloidal, N\'eel-type skyrmion lattice, as well as field-polarized ferromagnetic phases below 13 K. At zero and small magnetic fields two collective modes are found at 5 and 15 GHz, which are characteristic of the cycloidal state in this easy-axis magnet. In finite fields, entering the skyrmion lattice phase, the spectrum transforms into a multi-mode pattern with absorption peaks near 4, 8, and 15 GHz. The spin excitation spectra in GaV$_4$S$_8$ and their field dependencies are found to be in close relation to those observed in materials with Bloch-type skyrmions. Distinct differences arise from the strong uniaxial magnetic anisotropy of GaV4S8 not present in so-far known skyrmion hosts

Anisotropic Exchange in LiCu2O2{\bf LiCu_2O_2}

We investigate the magnetic properties of the multiferroic quantum-spin system LiCu$_2$O$_2$ by electron spin resonance (ESR) measurements at $X$- and $Q$-band frequencies in a wide temperature range $(T_{\rm N1} \leq T \leq 300$\,K). The observed anisotropies of the $g$ tensor and the ESR linewidth in untwinned single crystals result from the crystal-electric field and from local exchange geometries acting on the magnetic Cu$^{2+}$ ions in the zigzag-ladder like structure of LiCu$_2$O$_2$. Supported by a microscopic analysis of the exchange paths involved, we show that both the symmetric anisotropic exchange interaction and the antisymmetric Dzyaloshinskii-Moriya interaction provide the dominant spin-spin relaxation channels in this material.Comment: 10 pages, 10 Figure

Role of alkaline metal in the rare-earth triangular antiferromagnet KYbO2_2

We report crystal structure and magnetic behavior of the triangular antiferromagnet KYbO$_2$, the A-site substituted version of the quantum spin liquid candidate NaYbO$_2$. The replacement of Na by K introduces an anisotropic tensile strain with 1.6% in-plane and 12.1% out-of-plane lattice expansion. Compared to NaYbO$_2$, both Curie-Weiss temperature and saturation field are reduced by about 20% as the result of the increased Yb--O--Yb angles, whereas the $g$-tensor of Yb$^{3+}$ becomes isotropic with $g=3.08(3)$. Field-dependent magnetization shows the plateau at 1/2 of the saturated value and suggests the formation of the up-up-up-down field-induced order in the triangular AYbO$_2$ oxides (A = alkali metal), in contrast to the isostructural selenides that exhibit the 1/3 plateau and the up-up-down field-induced order

Evidence for a Ru4+^{4+} Kondo Lattice in LaCu3_3Ru4_4O12_{12}

Rare $d$-electron derived heavy-fermion properties of the solid-solution series LaCu$_3$Ru$_x$Ti$_{4-x}$O$_{12}$ were studied for $1 \leq x \leq 4$ by resistivity, susceptibility, specific-heat measurements, and magnetic-resonance techniques. The pure ruthenate ($x = 4$) is a heavy-fermion metal characterized by a resistivity proportional to $T^2$ at low temperatures $T$. The coherent Kondo lattice formed by the localized Ru 4$d$ electrons is screened by the conduction electrons leading to strongly enhanced effective electron masses. By increasing titanium substitution the Kondo lattice becomes diluted resulting in single-ion Kondo properties like in the paradigm $4f$-based heavy-fermion compound Ce$_x$La$_{1-x}$Cu$_{2.05}$Si$_2$ [M. Ocko {\em et al.}, Phys. Rev. B \textbf{64}, 195106 (2001)]. In LaCu$_3$Ru$_x$Ti$_{4-x}$O$_{12}$ the heavy-fermion behavior finally breaks down on crossing the metal-to-insulator transition close to $x = 2$.Comment: 9 pages, 8 figure

Magnetic and vibrational properties of the covalent chain antiferromagnet RbFeS2

Ternary rubidium-iron sulfide, RbFeS2, belongs to a family of quasi-one-dimensional compounds with the general chemical composition AFeCh2 (where A – K, Rb, Cs, Tl; Ch – S, Se). Understanding the magnetic properties of these compounds is a challenge. The controversy concerning the spin-state of the iron ion needs to be resolved to build the proper model of magnetism. Single crystals of RbFeS2 were grown and characterized by powder x-ray diffraction. QD MPMS-5 SQUID magnetometry was used to measure the magnetic susceptibility, and specific heat was measured utilizing QD PPMS-9 setup. Above the transition to three-dimensional antiferromagnetic order at the Néel temperature of TN = 188 K, the susceptibility exhibits unusual quasi-linear increase up to the highest measured temperature of 500 K. The specific heat was measured in the temperature range 1.8 – 300 K. Ab initio phonon dispersion and density-of-states calculations were performed by means of density functional theory (DFT), and the calculated lattice specific heat was subtracted from the measured one giving the magnetic contribution to the specific heat. Our results suggest that the features of the magnetic specific heat are general for the whole family of the covalent chain ternary iron chalcogenides of the AFeCh2 structure and indicate an intermediate S = 3/2 spin state of the iron ion