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A. Loidl

Publications and source records attributed to A. Loidl.

At least 235 records · Page 13Linked to original sources
arXiv2005

Glassy freezing of orbital dynamics in FeCr2S4 and FeSc2S4

We report on a thorough dielectric investigation of the glass-like freezing of the orbital reorientation-dynamics, recently found for the crystalline sulpho-spinels FeCr2S4 and FeSc2S4. As the orbital reorientations are coupled to a rearrangement of the surrounding ionic lattice via the Jahn-Teller effect, the freezing of the orbital moments is revealed by a relaxational behaviour of the complex dielectric permittivity. Additional conductivity (both dc and ac) and contact contributions showing up in the spectra are taken into account by an equivalent circuit description. The orbital relaxation dynamics continuously slows down over six decades in time, before at the lowest temperatures the glass transition becomes suppressed by quantum tunnelling.

cond-mat.dis-nn↗
arXiv2005

Terahertz Conductivity at the Verwey Transition in Magnetite

The complex conductivity at the (Verwey) metal-insulator transition in Fe_3O_4 has been investigated at THz and infrared frequencies. In the insulating state, both the dynamic conductivity and the dielectric constant reveal a power-law frequency dependence, the characteristic feature of hopping conduction of localized charge carriers. The hopping process is limited to low frequencies only, and a cutoff frequency nu_1 ~ 8 meV must be introduced for a self-consistent description. On heating through the Verwey transition the low-frequency dielectric constant abruptly decreases and becomes negative. Together with the conductivity spectra this indicates a formation of a narrow Drude-peak with a characteristic scattering rate of about 5 meV containing only a small fraction of the available charge carriers. The spectra can be explained assuming the transformation of the spectral weight from the hopping process to the free-carrier conductivity. These results support an interpretation of Verwey transition in magnetite as an insulator-semiconductor transition with structure-induced changes in activation energy.

cond-mat.str-el↗
arXiv2005

Relaxor ferroelectricity and colossal magnetocapacitive coupling in ferromagnetic CdCr2S4

Multiferroic materials, which reveal magnetic and electric order, are in the focus of recent solid state research. Especially the simultaneous occurrence of ferroelectricity and ferromagnetism, combined with an intimate coupling of magnetization and polarization via magneto-capacitive effects, could pave the way for a new generation of electronic devices. Here we present measurements on a simple cubic spinel with unusual properties: It shows ferromagnetic order and simultaneously relaxor ferroelectricity, i.e. a ferroelectric cluster state, reached by a smeared-out phase transition, both with sizable ordering temperatures and moments. Close to the ferromagnetic ordering temperature the magneto-capacitive coupling, characterized by a variation of the dielectric constant in an external magnetic field, reaches colossal values of nearly 500%. We attribute the relaxor properties to geometric frustration, which is well known for magnetic moments, but here is found to impede long-range order of the structural degrees of freedom.

cond-mat.str-el↗
arXiv2005

Glassy Aging Dynamics

We present time-dependent dielectric loss data at different frequencies for a variety of glass formers after cooling below the glass temperature. The observed aging dynamics is described using a modified Kohlrausch-Williams-Watts law, which takes into account the time-dependent variation of the relaxation time during aging. It leads to values for the aging relaxation time and stretching exponent that are fully consistent with the results from equilibrium measurements performed at higher temperatures. Irrespective of the dynamic process prevailing in the investigated frequency region, the aging dynamics is always determined by the structural relaxation process.

cond-mat.dis-nn↗
arXiv2005

Heat capacity of the quantum magnet TiOCl

Measurements of the heat capacity C(T,H) of the one-dimensional quantum magnet TiOCl are presented for temperatures 2K < T < 300K and magnetic fields up to 5T. Distinct anomalies at 91K and 67K signal two subsequent phase transitions. The lower of these transitions clearly is of first order and seems to be related to the spin degrees of freedom. The transition at 92K probably involves the lattice and/or orbital moments. A detailed analysis of the data reveals that the entropy change through both transitions is surprisingly small (~ 0.1R), pointing to the existence strong fluctuations well into the non-ordered high-temperature phase. No significant magnetic field dependence was detected.

cond-mat.str-el↗
arXiv2004

Study of one-dimensional nature of (Sr,Ba)_2Cu(PO_4)_2 and BaCuP_2O_7 via 31P NMR

The magnetic behavior of the low-dimensional phosphates (Sr,Ba)_2 Cu(PO_4)_2 and BaCuP_2O_7 was investigated by means of magnetic susceptibility and ^{31}P nuclear magnetic resonance (NMR) measurements. We present here the NMR shift K(T), the spin-lattice 1/T_1 and spin-spin 1/T_2 relaxation-rate data over a wide temperature range 0.02 K < T < 300 K. The T-dependence of the NMR K(T) is well described by the S=1/2 Heisenberg antiferromagnetic chain model with an intrachain exchange of J/k_B = 165 K, 151 K, and 108 K in Sr_2Cu(PO_4)_2, Ba_2Cu(PO_4)_2, and BaCuP_2O_7, respectively. Our measurements suggest the presence of magnetic ordering at 0.8 K in BaCuP_2O_7 (J/k_B = 108 K). For all the samples, we find that 1/T_1 is nearly T-independent at low-temperatures (1 K < T < 10 K), which is theoretically expected for 1D chains when relaxation is dominated by fluctuations of the staggered susceptibility. At high temperatures, 1/T_1 varies nearly linearly with temperature.

cond-mat.str-el↗
arXiv2004

Anisotropy of the paramagnetic susceptibility in LaTiO$_{3}$: The electron-distribution picture in the ground state

The energy-level scheme and wave functions of the titanium ions in LaTiO$_{3}$ are calculated using crystal-field theory and spin-orbit coupling. The theoretically derived temperature dependence and anisotropy of the magnetic susceptibility agree well with experimental data obtained in an untwinned single crystal. The refined fitting procedure reveals an almost isotropic molecular field and a temperature dependence of the van Vleck susceptibility. The charge distribution of the 3d--electron on the Ti positions and the principle values of the quadrupole moments are derived and agree with NMR data and recent measurements of orbital momentum $ $ and crystal-field splitting. The low value of the ordered moment in the antiferromagnetic phase is discussed.

cond-mat.str-el↗
arXiv2004

Orbital Glass in FeCr2S4

Low-temperature heat-capacity investigations on the spinel FeCr2S4 with ferrimagnetic spin order and orbitally degenerated Jahn-Teller active Fe2+ ions in a tetrahedral crystal field, provide experimental evidence of an orbital liquid state above 10 K. We demonstrate that the low-temperature transition at 10 K arises from orbital order and is very sensitive to fine tuning of the stoichiometry in polycrystals. In single crystals the orbital order is fully suppressed resulting in an orbital glass state with the heat capacity following a strict T^2 dependence as temperature approaches zero.

cond-mat.str-el↗
arXiv2004

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.

cond-mat.dis-nn↗
arXiv2004

Cooperative dynamics in doped manganite films: phonon anomalies in the ferromagnetic state

We present optical measurements of phononic excitations in La$_{2/3}$Ca$_{1/3}$MnO$_{3}$ (LCMO) and La$_{2/3}$Sr$_{1/3}$MnO$_{3}$ (LSMO) thin films covering the full temperature range from the metallic ferromagnetic to the insulating paramagnetic phase. All eight phonons expected for the R$\bar{3}$c symmetry in LSMO and 17 out of the expected 25 phonons for the Pnma symmetry in LCMO have been determined. Close to the ferromagnetic-to-paramagnetic transition both compounds reveal an anomalous behavior but with different characteristics. Anomalies in the phononic spectra are a manifestation of the coupling of lattice degrees of freedom (DOF) to electronic DOF. Specifically, the low-frequency external group proves to be an indicator for lattice modifications induced by electronic correlations. The enhanced electron-phonon coupling in LCMO is responsible for Fano-like interference effects of distinct phonon modes with electronic continuum excitations: we observe asymmetric phonon line shapes, mode splitting and spectral weight transfer between modes.

cond-mat.str-el↗
arXiv2004

Phonon-Metamorphosis in Ferromagnetic Manganite Films: Probing the Evolution of an Inhomogeneous State

The analysis of phonon anomalies provides valuable information about the cooperative dynamics of lattice, spin and charge degrees of freedom. Significant is the anomalous temperature dependence of the external modes observed in La$_{2/3}$Sr$_{1/3}$MnO$_{3}$ (LSMO) films. The two external modes merge close to the ferromagnetic to paramagnetic transition at $T_C$ and, moreover, two new modes evolve in this temperature range with strong resonances at slightly higher frequencies. We propose that this observed phonon metamorphosis probes the inhomogeneous Jahn-Teller distortion, manifest on the temperature scale $T_C$. The analysis is based on the first observation of all eight phonon modes in the metallic phase of LSMO and on susceptibility measurements which identify a Griffiths-like phase.

cond-mat.str-el↗
arXiv2004

'Boson peak' and high-frequency excitations in glassy crystals

The high-frequency excitations in glasses and supercooled liquids belong to the great mysteries of the physics of condensed matter. While the fast process, located at GHz-THz, can be interpreted as encaged molecular motion, the occurrence of the boson peak (BP), dominating at THz frequencies, still is controversially debated. Two scenarios have evolved during recent years: the BP is truly collective in nature or, alternatively, it results from localized modes. To help solving this controversy, we have investigated the high-frequency dielectric loss of plastic crystals (PCs), having long-range translational but no orientational order. Having in mind the well-defined phonon modes in PCs compared to canonical glasses, and the infrared silence of acoustic phonon modes, millimeter-wave and far-infrared spectroscopy should provide valuable hints on the true origin of the BP. Here we show that PCs exhibit a BP-like feature with markedly different spectral shape compared to canonical glasses, evidencing that mixing of collective phonon with local relaxational modes causes the BP. In addition, we find clear evidence for a fast process also in PCs.

cond-mat.soft↗
arXiv2004

Non-intrinsic origin of the Colossal Dielectric Constants in CaCu3Ti4O12

The dielectric properties of CaCu3Ti4O12, a material showing colossal values of the dielectric constant, were investigated in a broad temperature and frequency range extending up to 1.3 GHz. A detailed equivalent circuit analysis of the results and two crucial experiments, employing different types of contacts and varying sample thickness, provide clear evidence that the apparently high values of the dielectric constant in CaCu3Ti4O12 are non-intrinsic and due to electrode polarization effects. The intrinsic properties of CaCu3Ti4O12 are characterized by charge transport via hopping of localized charge carriers and a relatively high dielectric constant of the order of 100.

cond-mat.mtrl-sci↗
arXiv2004

Complex interplay of 3d and 4f magnetism in La:GdMnO3

We report on structural, magnetic, electrical, and thermodynamic properties of Gd-doped LaMnO3 single crystals for Gd doping levels 0 <= x <= 1. At room temperature, for all doping levels the orthorhombic O' phase is indicative for a strong Jahn-Teller distortion. All compositions are insulating. The magnetism of La$_{1-x}$Gd$_x$MnO$_3$ is dominated by the relatively strong Mn-Mn exchange. The weakening of the antiferromagnetic interactions due to the significant decrease f the Mn-O-Mn bond angles leads to the continuous suppression of the magnetic phase-transition temperatures into the antiferromagnetic low-temperature phase for increasing Gd doping. The magnetization can only be explained assuming canting of the manganese spins. The magnetic moments of Gd are weakly antiferromagnetically coupled within the sublattice and are antiferromagnetically coupled to the Mn moments. For intermediate concentrations compensation points are found, below which the spontaneous magnetization becomes negative. In pure GdMnO3 the Mn spins undergo a transition into a complex, probably incommensurate magnetic structure at 41.5 K, followed by a further ordering transition at 16-20 K revealing weak ferromagnetism due to canting and finally by the onset of magnetic order in the Gd sublattice at 6.5 K. At the lowest temperatures and low external fields both magnetic sublattices reveal a canted structure with antiparallel ferromagnetic components.

cond-mat.str-el↗
arXiv2004

Spin and orbital frustration in MnSc_2S_4 and FeSc_2S_4

Crystal structure, magnetic susceptibility, and specific heat were measured in the normal cubic spinel compounds MnSc_2S_4 and FeSc_2S_4. Down to the lowest temperatures, both compounds remain cubic and reveal strong magnetic frustration. Specifically the Fe compound is characterized by a Curie-Weiss temperature Θ_{CW}= -45 K and does not show any indications of order down to 50 mK. In addition, the Jahn-Teller ion Fe^{2+} is orbitally frustrated. Hence, FeSc_2S_4 belongs to the rare class of spin-orbital liquids. MnSc_2S_4 is a spin liquid for temperatures T > T_N \approx 2 K.

cond-mat.str-el↗
arXiv2004

Spin fluctuations in the quasi-two dimensional Heisenberg ferromagnet GdI_2 studied by Electron Spin Resonance

The spin dynamics of GdI_2 have been investigated by ESR spectroscopy. The temperature dependences of the resonance field and ESR intensity are well described by the model for the spin susceptibility proposed by Eremin et al. [Phys. Rev. B 64, 064425 (2001)]. The temperature dependence of the resonance linewidth shows a maximum similar to the electrical resistance and is discussed in terms of scattering processes between conduction electrons and localized spins.

cond-mat.str-el↗
arXiv2003

Magnetic and thermodynamic properties of RMnO$_3$ (R = Pr, Nd)

The ground state properties of the pure perovskite compounds PrMnO$_3$ and NdMnO$_3$ were investigated by magnetization, magnetic AC susceptibility and specific heat measurements. A strongly anisotropic behavior has been detected for temperatures below the antiferromagnetic phase transition $T_N$~100K. The susceptibility and the weak spontaneous ferromagnetic moment appear to be different in both compounds due to different anisotropic rare earth contributions. The specific heat shows strong Schottky type contributions at low temperatures, which for NdMnO$_3$ strongly depend on the magnetic field. A spin reorientation phase transition (spin-flop type) induced by a magnetic field along b axis was observed in NdMnO$_3$ at H~110kOe and T=5K. All results can consistently be explained by anisotropic contributions of the rare earth ions: In PrMnO$_3$ the electronic ground state is determined by a low lying quasidoublet split by the crystal field ~19 K. In NdMnO$_3$ the Kramers doublet is split by an exchange Nd-Mn field (~20K).

cond-mat↗