arXiv subjects

A. Loidl

Publications and source records attributed to A. Loidl.

At least 37 records · Page 2Linked to original sources

arXiv2019

Johari-Goldstein relaxation in glass-electrets

We investigate the dielectric response in the glass-electret state of two dipolar glass-forming materials. This unusual polar glassy state of matter is produced when a dipolar liquid is supercooled under the influence of a high electric dc field, which leads to partial orientational order of the molecules carrying a dipole moment. Investigation of the prepared glass-electrets by using low-field dielectric spectroscopy reveals a clear modification of their dielectric response in the regime of the Johari-Goldstein beta-relaxation, pointing to a small but significant increase of its relaxation strength compared to the normal glass. We discuss the implications of this finding for the still controversial microscopic interpretation of the Johari-Goldstein relaxation, an inherent property of glassy matter.

cond-mat.dis-nn↗

arXiv2019

Spin-lattice coupling in a ferrimagnetic spinel: The exotic $H$-$T$ phase diagram of MnCr$_2$S$_4$ up to 110 T

In antiferromagnets, the interplay of spin frustration and spin-lattice coupling has been extensively studied as the source of complex spin patterns and exotic magnetism. Here, we demonstrate that, although neglected in the past, the spin-lattice coupling is essential to ferrimagnetic spinels as well. We performed ultrahigh-field magnetization measurements up to 110 T on a Yafet-Kittel ferrimagnetic spinel, MnCr$_2$S$_4$, which was complemented by measurements of magnetostriction and sound velocities up to 60 T. Classical Monte Carlo calculations were performed to identify the complex high-field spin structures. Our minimal model incorporating spin-lattice coupling accounts for the experimental results and corroborates the complete phase diagram, including two new high-field phase transitions at 75 and 85 T. Magnetoelastic coupling induces striking effects: An extremely robust magnetization plateau is embedded between two unconventional spin-asymmetric phases. Ferrimagnetic spinels provide a new platform to study asymmetric and multiferroic phases stabilized by spin-lattice coupling.

cond-mat.str-el↗

arXiv2019

Hertz-to-terahertz dielectric response of nanoconfined water molecules

Broad-band dielectric spectroscopy, heat capacity measurements and molecular dynamic simulations are applied to study excitations of interacting electric dipoles spatially arranged in a network with an inter-dipole distance of 5-10 A. The dipoles with magnitude of 1.85 Debye are represented by single H2O molecules located in voids (0.5 nm size) formed by ions of the crystal lattice of cordierite. We discover emergence of nontrivial disordered paraelectric phase of dipolar system with signs of phase transition below 3 K.

cond-mat.mtrl-sci↗

arXiv2019

Structure, superconductivity, and magnetism in Rb1-xFe1.6Se2-zSz

The single-crystal growth, stoichiometry, and structure of Rb1-xFe2-ySe2-zSz crystals with substitution of Se by S are reported. The variation of the magnetic and thermodynamic parameters of samples was studied by differential-scanning calorimetry, magnetic susceptibility, conductivity, and specific heat. The experimental results are discussed within a T-z phase diagram, which includes vacancy-ordered and vacancy-disordered antiferromagnetic (AFM), superconducting (SC), and non-superconducting phases. The structural study revealed change in the local environment of the Fe tetrahedrons depending on substitution: a reduction of the Fe-Fe and Fe-Ch(chalcogen) bond lengths and a tendency for the six out of eight bond angles to approach values for a regular tetrahedron suggesting a reduction of structural distortions with substitution. With increasing substitution, a lowering of the superconducting transition temperature Tc was observed; the percolation threshold for the SC state is located at the substitution z = 1.2. The SC state was found to coexist with the AFM state that persists in all samples independent of substitution. The temperature of the transition into the AFM state TN shows a monotonous decrease indicating a weakening of the AFM interactions with increasing substitution. The AFM phase exhibits an iron-vacancy-ordered structure below the structural transition at Ts. The temperature Ts shows a non-monotonous variation: a decrease with increasing z up to 1.3, followed by an increase for further increasing z. The suppression of the superconductivity with substitution is accompanied by a significant reduction of the density of states at the Fermi energy and a weakening of the electronic correlations in the studied system.

cond-mat.supr-con↗

arXiv2019

High-Field Quantum Disordered State in $α$-RuCl3: Spin Flips, Bound States, and a Multi-Particle Continuum

Layered $α$-RuCl3 has been discussed as a proximate Kitaev spin liquid compound. Raman and THz spectroscopy of magnetic excitations confirm that the low-temperature antiferromagnetic ordered phase features a broad Raman continuum, together with two magnon-like excitations at 2.7 and 3.6 meV, respectively. The continuum strength is maximized as long-range order is suppressed by an external magnetic field. The state above the field-induced quantum phase transition around 7.5 T is characterized by a gapped multi-particle continuum out of which a two-particle bound state emerges, together with a well-defined single-particle excitation at lower energy. Exact diagonalization calculations demonstrate that Kitaev and off-diagonal exchange terms in the Fleury-Loudon operator are crucial for the occurrence of these features in the Raman spectra. Our study firmly establishes the partially-polarized quantum disordered character of the high-field phase.

cond-mat.str-el↗

arXiv2019

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.

cond-mat.dis-nn↗

arXiv2019

Spin relaxation in Cs$_2$CuCl$_{4-x}$Br$_x$

The quantum-spin S = 1=2 chain system Cs$_2$CuCl$_4$ is of high interest due to competing anti-ferromagnetic intra-chain J and inter-chain exchange J' interactions and represents a paramount example for Bose-Einstein condensation of magnons [R. Coldea et al., Phys. Rev. Lett. 88, 137202 (2002)]. Substitution of chlorine by bromine allows tuning the competing exchange interactions and corresponding magnetic frustration. Here we report on electron spin resonance (ESR) in single crystals of Cs$_2$CuCl$_{4-x}$Br$_x$ with the aim to analyze the evolution of anisotropic exchange contributions. The main source of the ESR linewidth is attributed to the uniform Dzyaloshinskii-Moriya interaction. The vector components of the Dzyaloshinskii-Moriya interaction are determined from the angular dependence of the ESR spectra using a high-temperature approximation. The obtained results support the site selectivity of the Br substitution suggested from the evolution of lattice parameters and magnetic susceptibility dependent on the Br concentration.

cond-mat.str-el↗

arXiv2019

Quantum Critical Dynamics of a Heisenberg-Ising Chain in a Longitudinal Field: Many-Body Strings versus Fractional Excitations

We report a high-resolution terahertz spectroscopic study of quantum spin dynamics in the antiferromagnetic Heisenberg-Ising spin-chain compound BaCo$_2$V$_2$O$_8$ as a function of temperature and longitudinal magnetic field. Confined spinon excitations are observed in an antiferromagnetic phase below $T_N\simeq 5.5$ K. In a field-induced gapless phase above $B_c=3.8$ T, we identify many-body string excitations as well as low-energy fractional psinon/antipsinon excitations by comparing to Bethe-Ansatz calculations. In the vicinity of $B_c$, the high-energy string excitations are found to be dynamically dominant over the fractional excitations.

cond-mat.str-el↗

arXiv2019

THz excitations in α-RuCl3: Majorana fermions, rigid-plane shear and compression modes

Spin liquids may host emergent quasiparticles, collective excitations of the spin degrees of freedom with characteristic features of Majorana fermions, which experimentally are detectable by broad excitation continua due to spin fractionalization. The latter is predicted for the Kitaev spin liquid, an exactly solvable model with bond-dependent interactions on a two-dimensional honeycomb lattice. Here we report on detailed THz experiments in α-RuCl3, identifying these characteristic fingerprints of Majorana fermions. The continuum intensity decreases and finally vanishes on increasing temperature. It partly overlaps with phonon modes representing characteristic sliding and compression modes of the van der Waals bonded molecular layers.

cond-mat.str-el↗

arXiv2019

Ionic conductivity of deep eutectic solvents: The role of orientational dynamics and glassy freezing

We have performed a thorough examination of the reorientational relaxation dynamics and the ionic charge transport of three typical deep eutectic solvents, ethaline, glyceline and reline by broadband dielectric spectroscopy. Our experiments cover a broad temperature range from the low-viscosity liquid down to the deeply supercooled state, allowing to investigate the significant influence of glassy freezing on the ionic charge transport in these systems. In addition, we provide evidence for a close coupling of the ionic conductivity in these materials to reorientational dipolar motions which should be considered when searching for deep eutectic solvents optimized for electrochemical applications.

cond-mat.soft↗

arXiv2019

Glycerol confined in zeolitic imidazolate frameworks: The temperature-dependent cooperativity length scale of glassy freezing

In the present work, we employ broadband dielectric spectroscopy to study the molecular dynamics of the prototypical glass former glycerol confined in two microporous zeolitic imidazolate frameworks (ZIF-8 and ZIF-11) with well-defined pore diameters of 1.16 and 1.46 nm, respectively. The spectra reveal information on the modified alpha relaxation of the confined supercooled liquid, whose temperature dependence exhibits clear deviations from the typical super-Arrhenius temperature dependence of the bulk material, depending on temperature and pore size. This allows assigning well-defined cooperativity length scales of molecular motion to certain temperatures above the glass transition. We relate these and previous results on glycerol confined in other host systems to the temperature-dependent length scale deduced from nonlinear dielectric measurements. The combined experimental data can be consistently described by a critical divergence of this correlation length as expected within theoretical approaches assuming that the glass transition is due to an underlying phase transition.

cond-mat.dis-nn↗

arXiv2018

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.

cond-mat.str-el↗

arXiv2018

Thermodynamic evidence of fractionalized excitations in α-RuCl3

Fractionalized excitations are of considerable interest in recent condensed-matter physics. Fractionalization of the spin degrees of freedom into localized and itinerant Majorana fermions are predicted for the Kitaev spin liquid, an exactly solvable model with bond-dependent interactions on a two-dimensional honeycomb lattice. As function of temperature, theory predicts a characteristic two-peak structure of the heat capacity as fingerprint of these excitations. Here we report on detailed heat-capacity experiments as function of temperature and magnetic field in high-quality single crystals of α-RuCl3 and undertook considerable efforts to determine the exact phonon background. We measured single-crystalline RhCl3 as non-magnetic reference and performed ab-initio calculations of the phonon density of states for both compounds. These ab-initio calculations document that the intrinsic phonon contribution to the heat capacity cannot be obtained by a simple rescaling of the nonmagnetic reference using differences in the atomic masses. Sizable renormalization is required even for non-magnetic RhCl3 with its minute difference from the title compound. In α-RuCl3 in zero magnetic field, excess heat capacity exists at temperatures well above the onset of magnetic order. In external magnetic fields far beyond quantum criticality, when long-range magnetic order is fully suppressed, the excess heat capacity exhibits the characteristic two-peak structure. In zero field, the lower peak just appears at temperatures around the onset of magnetic order and seems to be connected with canonical spin degrees of freedom. At higher fields, beyond the critical field, this peak is shifted to 10 K. The high-temperature peak located around 50 K is hardly influenced by external magnetic fields, carries the predicted amount of entropy, R/2 ln2, and may resemble remnants of Kitaev physics.

cond-mat.str-el↗

arXiv2018

Importance of reorientational dynamics for the charge transport in ionic liquids

Most ionic liquids contain at least one rather complex ion species exhibiting a dipolar moment. In the present work, we provide a thorough evaluation of broadband dielectric spectra of 12 ionic liquids taking into account the often neglected reorientational dynamics of these ions. We confirm that this dynamics leads to a clear relaxational signature in the spectra, a fact that so far only was considered in few previous works. The obtained reorientational relaxation times are well consistent with earlier inelastic light-scattering and high-frequency dielectric investigations. Evaluating our dielectric spectra in terms of reorientational motions reveals a close coupling of the ion-rotation dynamics to the ionic charge transport in a broad temperature range from the low-viscosity liquid above room temperature deep into the high-viscosity supercooled state close to Tg. This coupling does not seem to be mediated by the viscosity but probably is of more direct nature, pointing to a revolving-door mechanism as also considered for plastic-crystalline ionic conductors. Our results show that the reorientational motion of the dipolar ions plays a significant and so far widely overlooked role for the ionic charge transport in ionic liquids.

cond-mat.soft↗

arXiv2018

Third and Fifth Harmonic Responses in Viscous Liquids

We review the works devoted to third and fifth harmonic susceptibilities in glasses, namely $χ$ (3) 3 and $χ$ (5) 5. We explain why these nonlinear responses are especially well adapted to test whether or not some amorphous correlations develop upon cooling. We show that the experimental frequency and temperature dependences of $χ$ (3) 3 and of $χ$ (5) 5 have anomalous features, since their behavior is qualitatively different to that of an ideal gas, which is the high-temperature limit of a fluid. Most of the works have interpreted this anomalous behavior as reflecting the growth, upon cooling, of amorphously ordered domains, as predicted by the general framework of Bouchaud and Biroli (BB). We explain why most-if not all-of the challenging interpretations can be recast in a way which is consistent with that of Bouchaud and Biroli. Finally, the comparison of the anomalous features of $χ$ (5) 5 and of $χ$ (3) 3 shows that the amorphously ordered domains are compact, i.e., the fractal dimension d f is close to the dimension d of space. This suggests that the glass transition of molecular liquids corresponds to a new universality class of critical phenomena.

cond-mat.soft↗

arXiv2018

Sub-gap optical response across the structural phase transition in van der Waals layered α-RuCl$_3$

We report magnetic, thermodynamic, thermal expansion, and on detailed optical experiments on the layered compound $α$-RuCl$_3$ focusing on the THz and sub-gap optical response across the structural phase transition from the monoclinic high-temperature to the rhombohedral low-temperature structure, where the stacking sequence of the molecular layers is changed. This type of phase transition is characteristic for a variety of tri-halides crystallizing in a layered honeycomb-type structure and so far is unique, as the low-temperature phase exhibits the higher symmetry. One motivation is to unravel the microscopic nature of spin-orbital excitations via a study of temperature and symmetry-induced changes. We document a number of highly unusual findings: A characteristic two-step hysteresis of the structural phase transition, accompanied by a dramatic change of the reflectivity. An electronic excitation, which appears in a narrow temperature range just across the structural phase transition, and a complex dielectric loss spectrum in the THz regime, which could indicate remnants of Kitaev physics. Despite significant symmetry changes across the monoclinic to rhombohedral phase transition, phonon eigenfrequencies and the majority of spin-orbital excitations are not strongly influenced. Obviously, the symmetry of the single molecular layers determine the eigenfrequencies of most of these excitations. Finally, from this combined terahertz, far- and mid-infrared study we try to shed some light on the so far unsolved low energy (< 1eV) electronic structure of the ruthenium $4d^5$ electrons in $α$-RuCl$_3$.

cond-mat.str-el↗

arXiv2018

Quantum Criticality of an Ising-like Spin-1/2 Antiferromagnetic Chain in Transverse Magnetic Field

We report on magnetization, sound velocity, and magnetocaloric-effect measurements of the Ising-like spin-1/2 antiferromagnetic chain system BaCo$_2$V$_2$O$_8$ as a function of temperature down to 1.3 K and applied transverse magnetic field up to 60 T. While across the Néel temperature of $T_N\sim5$ K anomalies in magnetization and sound velocity confirm the antiferromagnetic ordering transition, at the lowest temperature the field-dependent measurements reveal a sharp softening of sound velocity $v(B)$ and a clear minimum of temperature $T(B)$ at $B^{c,3D}_\perp=21.4$ T, indicating the suppression of the antiferromagnetic order. At higher fields, the $T(B)$ curve shows a broad minimum at $B^c_\perp = 40$ T, accompanied by a broad minimum in the sound velocity and a saturation-like magnetization. These features signal a quantum phase transition which is further characterized by the divergent behavior of the Grüneisen parameter $Γ_B \propto (B-B^{c}_\perp)^{-1}$. By contrast, around the critical field, the Grüneisen parameter converges as temperature decreases, pointing to a quantum critical point of the one-dimensional transverse-field Ising model.

cond-mat.str-el↗

arXiv2018

Relaxation dynamics in the one-dimensional organic charge-transfer salt δ-(EDT-TTF-CONMe$_2$)$_2$Br

A detailed investigation of the charge-ordered charge-transfer salt δ-(EDT-TTF-CONMe$_{2}$)$_{2}$Br by thermal-expansion measurements and dielectric spectroscopy reveals three dynamic processes of relaxational character. The slowest one exhibits the characteristics of glassy freezing and is ascribed to the conformational dynamics of terminal ethylene groups of the organic molecules. Such a process was previously found for related charge-transfer salts where, however, the anions form polymerlike chains, in contrast to the spherical anions of the present material. Dielectric spectroscopy reveals two additional relaxational processes. The characteristics of the faster one are consistent with excitations of a one-dimensional Wigner lattice as recently observed in this material by infrared spectroscopy, which are also accompanied by conformational changes of the molecules. However, at low temperature the ethylene-group relaxation exhibits the cooperativity-induced dramatic slowing down that is typical for glassy freezing, while the defect-related Wigner-lattice excitation follows thermally activated behavior as expected for single-dipole relaxations.

cond-mat.str-el↗