α\alpha- and β\beta- Relaxation Dynamics of a fragile plastic crystal

We present a thorough dielectric investigation of the relaxation dynamics of plastic crystalline Freon112, which exhibits freezing of the orientational degrees of freedom into a glassy crystal below 90 K. Among other plastic crystals, Freon112 stands out by being relatively fragile within Angell's classification scheme and by showing an unusually strong $\beta$-relaxation. Comparing the results to those on Freon112a, having only a single molecular conformation, points to the importance of the presence of two molecular conformations in Freon112 for the explanation of its unusual properties.Comment: 17 pages, 6 figure

Low temperature dielectric relaxation study of aqueous solutions of diethylsulfoxide

In the present work, dielectric spectra of mixtures of diethylsulfoxide (DESO) and water are presented, covering a concentration range of 0.2 - 0.3 molar fraction of DESO. The measurements were performed at frequencies between 1 Hz and 10 MHz and for temperatures between 150 and 300 K. It is shown that DESO/water mixtures have strong glass-forming abilities. The permittivity spectra in these mixtures reveal a single relaxation process. It can be described by the Havriliak-Negami relaxation function and its relaxation times follow the Vogel-Fulcher-Tammann law, thus showing the typical signatures of glassy dynamics. The concentration dependence of the relaxation parameters, like fragility, broadening, and glass temperature, are discussed in detail.Comment: 20 pages, 5 figure

Evolution of magnetic states in frustrated diamond lattice antiferromagnetic Co(Al1-xCox)2O4 spinels

Using neutron powder diffraction and Monte-Carlo simulations we show that a spin-liquid regime emerges at $all compositions in the diamond-lattice antiferromagnets Co(Al1-xCox)2O4. This spin-liquid regime induced by frustration due to the second-neighbour exchange coupling J2, is gradually superseded by antiferromagnetic collinear long-range order (k=0) at low temperatures. Upon substitution of Al3+ by Co3+ in the octahedral B-site the temperature range occupied by the spin-liquid regime narrows and TN increases. To explain the experimental observations we considered magnetic anisotropy D or third-neighbour exchange coupling J3 as degeneracy-breaking perturbations. We conclude that Co(Al1-xCox)2O4 is below the theoretical critical point J2/J1=1/8, and that magnetic anisotropy assists in selecting a collinear long-range ordered ground state, which becomes more stable with increasing x due to a higher efficiency of O-Co3+-O as an interaction path compared to O-Al3+-O

Plastic-crystalline solid-state electrolytes: Ionic conductivity and orientational dynamics in nitrile mixtures

Many plastic crystals, molecular solids with long-range, center-of-mass crystalline order but dynamic disorder of the molecular orientations, are known to exhibit exceptionally high ionic conductivity. This makes them promising candidates for applications as solid-state electrolytes, e.g., in batteries. Interestingly, it was found that the mixing of two different plastic-crystalline materials can considerably enhance the ionic dc conductivity, an important benchmark quantity for electrochemical applications. An example is the admixture of different nitriles to succinonitrile, the latter being one of the most prominent plastic-crystalline ionic conductors. However, until now only few such mixtures were studied. In the present work, we investigate succinonitrile mixed with malononitrile, adiponitrile, and pimelonitrile, to which 1 mol% of Li ions were added. Using differential scanning calorimetry and dielectric spectroscopy, we examine the phase behavior and the dipolar and ionic dynamics of these systems. We especially address the mixing-induced enhancement of the ionic conductivity and the coupling of the translational ionic mobility to the molecular reorientational dynamics, probably arising via a "revolving-door" mechanism.Comment: 9 pages, 7 figures; revised version as accepted for publication in J. Chem. Phy

Spin-orbiton and quantum criticality in FeSc2S4

In FeSc2S4 spin-orbital exchange competes with strong spin-orbit coupling, suppressing long-range spin and orbital order and, hence, this material represents one of the rare examples of a spin-orbital liquid ground state. Moreover, it is close to a quantum-critical point separating the ordered and disordered regimes. Using THz and FIR spectroscopy we study low-lying excitations in FeSc2S4 and provide clear evidence for a spin-orbiton, an excitation of strongly entangled spins and orbitals. It becomes particularly well pronounced upon cooling, when advancing deep into the quantum-critical regime. Moreover, indications of an underlying structureless excitation continuum are found, a possible signature of quantum criticality.Comment: 11 pages, 11 figures (including 4 pages and 5 figures in Supplemental Material). Revised version according to suggestions of referees. Phys. Rev. B (in press

Characteristics of ferroelectric-ferroelastic domains in N{\'e}el-type skyrmion host GaV4_4S8_8

GaV$_4$S$_8$ is a multiferroic semiconductor hosting N{\'e}el-type magnetic skyrmions dressed with electric polarization. At T$_s$ = 42K, the compound undergoes a structural phase transition of weakly first-order, from a non-centrosymmetric cubic phase at high temperatures to a polar rhombohedral structure at low temperatures. Below T$_s$, ferroelectric domains are formed with the electric polarization pointing along any of the four $\left< 111 \right>$ axes. Although in this material the size and the shape of the ferroelectric-ferroelastic domains may act as important limiting factors in the formation of the N{\'e}el-type skyrmion lattice emerging below T$_C$=13\:K, the characteristics of polar domains in GaV$_4$S$_8$ have not been studied yet. Here, we report on the inspection of the local-scale ferroelectric domain distribution in rhombohedral GaV$_4$S$_8$ using low-temperature piezoresponse force microscopy. We observed mechanically and electrically compatible lamellar domain patterns, where the lamellae are aligned parallel to the (100)-type planes with a typical spacing between 100 nm-1.2 $\mu$m. We expect that the control of ferroelectric domain size in polar skyrmion hosts can be exploited for the spatial confinement and manupulation of N{\'e}el-type skyrmions

Weak ferromagnetism and glassy state in kappa-(BEDT-TTF)2Hg(SCN)2Br

Since the first observation of weak ferromagnetism in the charge-transfer salt kappa-(BEDT-TTF)2-Cu[N(CN)2]Cl [U. Welp et al., Phys. Rev. Lett. 69, 840 (1992)], no further evidence of ferromagnetism in this class of organic materials has been reported. Here we present static and dynamic spin susceptibility measurements on kappa-(BEDT-TTF)2Hg(SCN)2Br revealing weak ferromagnetism below about TWF = 20 K. We suggest that frustrated spins in the molecular dimers suppress long-range order, forming a spin-glass ground state in the insulating phase

Magnetic ground state and 2D behavior in pseudo-Kagome layered system Cu3Bi(SeO3)2O2Br

Anisotropic magnetic properties of a layered kagome-like system Cu3Bi(SeO3)2O2Br have been studied by bulk magnetization and magnetic susceptibility measurements as well as powder and single-crystal neutron diffraction. At T_N = 27.4 K the system develops an alternating antiferromagnetic order of (ab) layers, which individually exhibit canted ferrimagnetic moment arrangement, resulting from the competing ferro- and antiferro-magnetic intralayer exchange interactions. A magnetic field B_C ~ 0.8 T applied along the c axis (perpendicular to the layers) triggers a metamagnetic transition, when every second layer flips, i.e., resulting in a ferrimagnetic structure. Significantly higher fields are required to rotate the ferromagnetic component towards the b axis (~7 T) or towards the a axis (~15 T). The estimates of the exchange coupling constants and features indicative of an XY character of this quasi-2D system are presented.Comment: 7 pages, 6 figures, final versio

Anisotropic Exchange in LiCuVO4_4 probed by ESR

We investigated the paramagnetic resonance in single crystals of LiCuVO$_4$ with special attention to the angular variation of the absorption spectrum. To explain the large resonance linewidth of the order of 1 kOe, we analyzed the anisotropic exchange interaction in the chains of edge-sharing CuO$_6$ octahedra, taking into account the ring-exchange geometry of the nearest-neighbor coupling via two symmetric rectangular Cu-O bonds. The exchange parameters, which can be estimated from theoretical considerations, nicely agree with the parameters obtained from the angular dependence of the linewidth. The anisotropy of this magnetic ring exchange is found to be much larger than it is usually expected from conventional estimations which neglect the bonding geometry. Hence, the data yield the evidence that in copper oxides with edge-sharing structures the role of the orbital degrees of freedom is strongly enhanced. These findings establish LiCuVO$_4$ as one-dimensional compound at high temperatures. PACS: 76.30.-v, 76.30.Fc, 75.30.EtComment: 18 pages, 6 figure