Magnetic properties of some rare‐earth magnesium compounds RMg2

The magnetic properties of the compounds PrMg2, NdMg2, DyMg2, and ErMg2 were studied by means of neutron diffraction at various temperatures. All these compounds give rise to ferromagnetic ordering. The absolute values of the magnetic moments in the magnetically ordered state are lower than the free‐ion values. Inelastic neutron scattering at several temperatures was studied in PrMg2 and NdMg2. Analysis of the scattering data in conjunction with the results of specific‐heat and magnetization measurements shows that PrMg2 is an induced‐moment system (G3 ground state), where quadrupolar effects carry a large weight in determining the magnetic properties. The values found for the crystal‐field…

Dielectric study of orientational disorder in (CO2)1−x(N2O)xmixed crystals

The dipolar relaxation dynamics of solid solutions of carbon dioxide and nitrous oxide has been investigated using dielectric spectroscopy. The temperature dependence of the relaxation rate reveals an ideal Arrhenius behavior for all concentrations, with energy barriers which scale linearly between the two pure compounds. The attempt frequencies are anomalously high. The distribution of relaxation times due to the static random fields as introduced by the substitutional impurity molecules is almost negligible. The melting temperature is determined by a critical relaxation rate of 40 kHz.

Ferroelastic transition in Kbr:Kcn studied by neutrons, x-rays and ultrasonic

The ferroelastic phase transition of (KBr) 0 27 (KNC) 0.73 has been studied by X-ray diffraction, ultrasonics and inelastic neutron scattering. It is the first example of a cubic crystal where the elastic shear constant C 44 softens completely corresponding to the m = 2 universality class. C 44 and the Bragg intensities show a non-classical critical behaviour.

Single particle jumps and correlated ionic motions in glass-ceramics

Using impedance spectroscopy, the ion transport in poorly Li-conducting aluminosilicate glass ceramics and their precursor glasses has been measured for temperatures 50 K < T < 550 K and covering a frequency range of more than 14 decades from 10 mHz up to 3 THz. In addition to the familiar cooperative ionic motion dominating at high temperatures, for the first time dielectric relaxation due to elementary hopping processes is observed well below room temperature.

Frequency Dependence of the Orientational Freezing in(KBr)1−x(KCN)x

Dielectric, ultrasonic, and neutron-scattering measurements in ${(\mathrm{KBr})}_{1\ensuremath{-}x}{(\mathrm{KCN})}_{x}$ are reported for concentrations $x$ ranging from 0.01 to 0.5. The dipolar and the quadrupolar susceptibilities exhibit frequency- and concentration-dependent cusps showing that the freezing process into an orientational glass state is a relaxational phenomenon.

Elastic properties of CsCN

The temperature dependence of the elastic constants of CsCN exhibiting the CsCl structure was measured with ultrasonic and neutron techniques. The room temperature values were found to bec11=18.8,c12=10.7 andc44=2.95 1010 dyn/cm2. The sound waves inT2g andEg symmetries exhibit anomalous temperature effects which are similar but definitively weaker than those in the NaCl type cyanides. In addition we measured the acoustic phonon dispersion along [100] and [110]. These results are compared with recent molecular dynamics calculations.

LOCAL-MOMENT AND ITINERANT ANTIFERROMAGNETISM IN THE HEAVY-FERMION SYSTEM CE(CU1-XNIX)2GE2

Elastic and inelastic neutron-scattering studies on the system Ce(Cu1−xNix)2Ge2 are reported. These measurements are complemented by measurements of the magnetic susceptibility, high-field magnetization, heat capacity, thermal expansion, electrical resistivity and thermopower. The results reveal an interesting T-x phase diagram consisting of two different antiferromagnetic phases for x 0.5. Further experimental evidence for different types of antiferromagnetic ordering derives from a line-shape analysis of the quasielastic neutron-scattering intensity, from magnetization and thermopower experiments.

Neutron-scattering studies on CeM2Ge2(M=Ag, Au, and Ru)

The results of elastic, quasielastic, and inelastic neutron-scattering studies on polycrystalline CeM 2 Ge 2 (M=Ag, Au, and Ru) are presented. All compounds reveal long-range magnetic order at low temperatures. Ferromagnetic (M=Ru), antiferromagnetic (M=Au), and incommensurate (M=Ag) structures were detected. Using time-of-flight (TOF) techniques, the crystalline electric-field splittings were determined. With high-resolution TOF experiments the temperature and wave-vector dependence of the magnetic relaxation rate was studied

Preparation, Characterisation and Dielectric Properties of YBa2Cu3O7-δ/ Insulator-Heterostructures

YBa 2 Cu 3 O 7-δ /insulator/Au-heterostructures on SrTiO 3 or LaAlO 3 substrates were prepared to study the properties of the materials SrTiO 3 , BaTiO 3 and Ceo 2 . X-ray diffraction measurements in Bragg-Brentano geometry show c-axis-oriented growth for the superconductor and the insulators SrTiO 3 and CeO 2 . Typical values for the rocking curve width of the different insulating films are between 0.4° and 0.8°. The highest breakdown fields are measured for the insulator SrTiO 3 with +37.5 kV/mm and -8.8 kV/mm. The permittivity for CeO 2 is independent of applied field and only weakly temperature dependent. This is in contrast to the perovskite type insulators, where the permittivity depe…

Quantum paraelectric and induced ferroelectric states in

Nominally pure has been studied by dielectric spectroscopy using small (linear regime) as well as large electrical fields (non-linear regime) up to . In addition measurements of the specific heat and its field-dependent contribution have been carried out. The field dependence of the dielectric constant and the specific heat can be well described by the transverse Ising Hamiltonian including tunnelling and external field terms. It gives evidence for the existence of polar clusters at low temperatures which are supposed to be associated with the quantum paraelectric state below in accord with recent free-energy calculations. The low-field third-harmonic susceptibility which measures the polar…

Frequency dependent conductivity in YBa2Cu3O7-δ (δ≈0) thin films

β-Relaxation and low-temperature specific heat in (KBr)1?x(KCN)x

The specific heat in (KBr)1−x(KCN)x has been measured for concentrations 0.00≦x≦0.93 and for temperatures 2 K≦T≦50 K. In addition, the dipolar relaxation phenomena were studied using dielectric spectroscopy. The relaxation behaviour was parametrized assuming a Gaussian distribution of energy barriers and the mean activation energies, the distribution widths, and the attempt frequencies have been determined as a function of the CN− concentration. With these parameters the linear and the excess specific heat contributions were calculated and compared to the calorimetric results.

Anisotropic exchange in ErSb

The correlations of the magnetic moments and the magnetic order parameter of ErSb have been studied by neutron diffraction. The antiferromagnetic phase transition is of first order. The diffuse paramagnetic scattering is evaluated in terms of magnetic coupling tensors which are characterized by a strong two-ion anisotropy.

ac conductivity inLa2CuO4

Measurements of the complex ac conductivity are reported for a single crystal of ${\mathrm{La}}_{2}$${\mathrm{CuO}}_{4}$ for frequencies ${10}^{2}$\ensuremath{\le}\ensuremath{\nu}\ensuremath{\le}${10}^{9}$ Hz and temperatures 25\ensuremath{\le}T\ensuremath{\le}300 K. The conductivity follows a power-law behavior ${\mathrm{\ensuremath{\omega}}}^{\mathit{s}}$ with the frequency exponent s independent of temperature and independent of frequency. However, the hopping transport is strongly anisotropic, with s\ensuremath{\approxeq}0.75 within the ${\mathrm{CuO}}_{2}$ planes and s\ensuremath{\approxeq}0.25 perpendicular to the planes.

Elastic constants in RbI, determined by inelastic neutron scattering

Long-wavelength acoustic phonons have been studied in the whole (100)-plane of RbI at 295 K by means of inelastic neutron scattering. The raw data have been corrected for resolution effects taking into account the curvature of the dispersion surface and variations of the mode eigenvectors. The shifts of the neutron groups due to these resolution effects are discussed in detail. The analysis of the experimental results gives for the zero sound elastic constantsc11=28.15±0.5,c12=3.7±0.5 andc44=2.85±0.1 1010 dyn/cm2. A comparison with first sound elastic constants taken from ultrasonic measurements yields significant differences between the high and low frequency elastic constantsc11 andc″=(c1…

Ion transport in the fragile glass former3KNO3-2Ca(NO3)2

The molten salt ${3\mathrm{K}\mathrm{N}\mathrm{O}}_{3}$-2Ca(${\mathrm{NO}}_{3}$${)}_{2}$ has been studied in the frequency range 5 mHz40 GHz and for temperatures 10 KT500 K using impedance spectroscopy. It is found that in the microwave regime the dynamic conductivity traces the primary response. In the radio- and audio-frequency ranges the mobile ion relaxation becomes increasingly decoupled and the time scale and stretching of the response as determined from electrical modulus spectra differ from those obtained by spectroscopies probing the structural response. For T\ensuremath{\gtrsim}360 K minima are detected in the dielectric loss that make possible a comparison with recent mode-coupli…

Broadband infrared conductivity in an YBa2Cu3O6.7 thin film

Infrared reflectivity of an oxygen reduced YBa2Cu3O6.7 thin film was measured in the frequency range 30 cm-1 < v < 7000 cm-1 and for temperatures 5 K < T < 300 K. At lower frequencies, 3 cm-1 < v < 40 cm-1, the complex conductivity σ*=σ1+iσ2 was measured directly using a transmission technique. Both data sets were combined to obtain the reflectivity in a broad frequency range and thus to improve substantially the quality of the Kramers-Kronig analysis at low frequencies. The analysis of the conductivity spectra reveals that the low-frequency spectral weight strongly depends on temperature directly above TC but saturates for T ≥ 150 K.

Magnetic order in a Kondo lattice: A neutron scattering study of CeCu2Ge2

Elastic and inelastic neutron scattering studies of the Kondo lattice CeCu2Ge2 were performed. AtTN=4.1 K an incommensurate magnetic order develops with an ordering wave vectorq0=(0.28, 0.28, 0.54) and an ordered moment µs=0.74 µB. The crystalline electric field splits the 4f1-J-multiplet of the Ce ion into a ground state doublet and a quartet at 191 K. The wave function of the ground state yields an ordered moment of 1.54µB. Thus, due to the onset of the formation of a Kondo singlet the magnetic moment is considerably reduced. The magnetic relaxation rate Λ was investigated via quasielastic neutron scattering. The temperature dependence of Λ(T) is characteristic of heavy-fermion systems wi…

Frequency-dependent conductivity of UPd2Al3 films

The transmission of UPd2Al3 films was studied (4 K < T < 300 K) in the frequency range from 4 to 32 cm−1 by using a coherent source interferometer which allows for measuring both, amplitude and phase. In addition we report on radio frequency and optical measurements. Below 20 K the conductivity and dielectric constant show strong deviations from the behavior of a normal metal which cannot simply be explained by a single renormalized Drude model with an enhanced mass and reduced scattering rate. Instead, we find evidence for the opening of a pseudogap with a gap energy of 6 cm−1 and an extremely narrow ω = 0 mode which is responsible for the large DC conductivity.

Hopping Conductivity in Hydrogen-Bonded Antiferroelectric Compounds

Antiferroelectric betaine phosphate (BP: (CH3)3NCH2COO · H3PO4) and ferroelectric betaine phosphite (BPI: (CH3)3NCH2COO · H3PO3) are molecular crystals of the amino acid betaine and the phosphoric or phosphorous acids, respectively. In both compounds the inorganic components are linked by hydrogen bonds to one-dimensional chains. The two isostructural compounds form solid solutions BPxBPI1-x at any concentration. Here we report measurements of the dielectric permittivity for concentrations 0.85 ≤ × ≤ 1 at frequencies 10−2 ≤ v ≤ 109 Hz and temperatures 2 K ≤ T ≤ 300 K. The dielectric response in BP:BPI (x = 0.95) is dominated by contributions from pure hopping conductivity which we ascribe t…

Alloying experiments on heavy fermion compounds

Abstract This paper is intended to demonstrate the usefulness of controlled alloying for the understanding of heavy-fermion physics: (1) Th-substitution for Ce in CeCu2Si2 emphasizes the dominating role of the dopant-induced strain fields in generating incoherent scattering and pair breaking, (2) replacement of Cu by Ni in Ce(Cu1-xNix)2Ge2 leads to phenomena which are interpreted as derived from a transition between local-moment and itinerant heavy-fermion magnetism, and (3) increasing Cu concentration in UCu4+xAl8-x is accompanied by an antiferromagnetic to nonmagnetic transition near xcr = 1.5 similar to what has been found before for several Ce-based systems. A heavy Fermi-liquid phase w…

On the phase transition in CsCN

X-ray diffraction and dielectric measurements have been performed on the molecular crystal CsCN as a function of temperature. The order parameter of the cubic to rhombohedral phase transition (Tc=186 K) was determined and interpreted by a coupling of the (CN)− orientations to the shear strain. At lower temperatures the dielectric response is dominated by thermally activated relaxations processes rather than by electrical ordering of the CN dipoles.

Dipolar and quadrupolar freezing in (NaCN)1−x(KCN)x

Instabilities in heavy-fermion systems

Abstract We review (i) an itinerant antiferromagnetic phase transition below 4 K in Ni-rich Ce(Cu 1− x Ni x ) 2 Ge 2 systems, (ii) the coincidence at T = 0.63 K of both a structural lattice instability in “as-grown” (non-superconducting) CeCu 2 Si 2 single crystals and bulk superconductivity in annealed ones as well as (iii) antiferromagnetic and superconducting transitions at T N = 4.6 K and T c = 1 K, respectively, in the heavy-fermion compound UNi 2 Al 3 .

Orientational glass behaviour of K Br0.96(CN)0.04

Ultrasonic measurements on the mixed crystal K Br0.96(CN)0.04 show a minimum of most of the elastic constants at 16 K. In addition we determinedc11(T) at 10 MHz and at 50 MHz observing dispersion effects. These results and previous Brillouin and neutron scattering results of other authors on higher CN-concentrations are interpreted by an orientational glass behaviour. A semiquantitative description is given in terms of the mean random field approximation.

Static freezing transition at a finite temperature in a quasi-one-dimensional deuteron glass.

The dipolar freezing process of a quasi-one-dimensional betaine deuteron glass was studied using linear and nonlinear dielectric spectroscopy. The linear response as measured for frequencies $5\mathrm{mHz}l\ensuremath{\nu}l200\mathrm{MHz}$ was analyzed using the recently invented $\ensuremath{\delta}$ plot, providing evidence for a static freezing transition near 30 K. Measurements of the ergodic to nonergodic transition as well as of the incipient divergence of the nonlinear susceptibility yield independent confirmation of this quasistatic freezing transition temperature. The critical exponent describing the nonlinear behavior is found to be $\ensuremath{\gamma}\phantom{\rule{0ex}{0ex}}=\p…

Ferroelasticity and glass-like behavior in alkali halide-alkali cyanide mixed crystals

Abstract Single crystal neutron diffraction studies in (KBr)1-x(KCN)x are summarized. Mixed crystals with CN− concentrations x > 0.6 exhibit ferroelastic phase transitions from a high-temperature plastic phase into a low-temperature elastically ordered phase in which the CN− orientations show long range orientational order and the center of mass lattice exhibits shear distortions. For concentrations x ≤ 0.6 orientational disorder is frozen-in and transitions into an orientational glass state occur. Close to the critical concentration xc ∼ 0.6 the diffraction profiles at the transition temperatures are dominated by diffuse-scattering contributions. These results are compared to model calcula…

Strong reduction of the Korringa relaxation in the spin-density wave regime ofEuFe2As2observed by electron spin resonance

Electron spin resonance measurements in ${\text{EuFe}}_{2}{\text{As}}_{2}$ single crystals revealed an absorption spectrum of a single resonance with Dysonian line shape. Above the spin-density wave (SDW) transition at ${T}_{\text{SDW}}=190\text{ }\text{K}$ the spectra are isotropic and the Eu spins relax via the conduction electrons resulting in a Korringa-type increase in the linewidth. Below ${T}_{\text{SDW}}$, a distinct anisotropy develops and the relaxation behavior of the Eu spins changes drastically into one with characteristic properties of a magnetic insulating system, where dipolar and crystal-field interactions dominate. This indicates a spatial confinement of the conduction ele…

Magnetic excitations in TbP under hydrostatic pressure

Singlet ground state magnets still attract much attention. In these systems magnetic ordering occurs via the polarization of the ground state, and noticeable dispersion of well defined excitations is expected in systems where the exchange coupling is about equal to the crystal field energy. In addition, the two singlet-triplet systems PrSbl and TbP2 where single crystals are available and which have been studied in detail showed a pronounced splitting of the Г1–Г4 magnetic excitations where the triple degeneracy was lifted along [100] and [011] by a strong anisotropy of the exchange.

Magnetic phase diagrams in heavy-fermion compounds

Magnetic phase diagrams have been explored in heavy-fermion (HF) compounds by controlled changes of the stoichiometry (UCu4+xAl8−x), dopant concentration (Ce(Cu1−xNix)2Ge2) and magnetic field (CeCu2Si2). The results demonstr competition (i) between Kondo and RKKY interactions in the former two compounds and (ii) between HF superconductivity and some cooperative state, presumably HF band magnetism, in the latter.

Relaxation dynamics in orientational glasses

Abstract The multipolar relaxation dynamics observed in dipolar and quadrupolar glasses are reviewed. Special attention is given to the distribution of the relaxation times and to the temperature dependence of the mean relaxation rates. Experimental evidence is provided that orientational glasses can be described in terms of ‘strong glasses’ that are characterized by a low density of configurational states in the potential energy surface. It is suggested that this behavior results from the natural separation of timescales of reorientational and diffusive processes in these crystals.

Ionic transport and heat capacity of glass-forming metalnitrate mixtures

Abstract Ionic transport of the glass-forming metalnitrate mixtures [Ca(NO 3 ) 2 ] 0.44 [KNO 3 ] 0.56 (MKN), and [Mg(NO 3 ) 2 ] 0.44 [NaNO 3 ] 0.56 (MNN) was investigated near the glass transition using broadband spectroscopy of the complex conductivity to 300 MHz. The real part of the conductivity exhibits a transition from frequency independent to power law behavior as found in most ionic conductors. At high frequencies the frequency exponent approaches unity and becomes larger at low temperatures. In the real part of the dielectric constant, a relaxation step could be observed in CRN. A detailed evaluation of the results within the modulus formalism is presented. The imaginary part of t…

Inelastic neutron scattering by coupled rotational and translational modes in KCN

The TA [100] phonon branch of the molecular crystal KCN was studied by inelastic neutron scattering in the cubic phase. In addition the distribution of the quasielastic scattered neutrons was investigated. The results are analysed by assuming a coupling of the phonon modes to the rotational degrees of freedom of the CN-dumb-bells which are regarded as a system of interacting quadrupoles. A good description of the present results and also of the existing ultrasonic and Brillouin data is achieved by a simple model which uses a single collective rotational mode of finite excitation energy and line width.

Coupled rotational and translational modes in the mixed molecular crystal KBr1?x (CN) x

TheE g andT 2g acoustic phonon modes of the molecular crystals KBr0.96(CN)0.04 and KBr0.86(CN)0.14 have been investigated by inelastic neutron scattering at 6, 90 and 300 K. Clear resonances due to mode-mode coupling to molecular excitations were observed. In complementary ultrasonic experiments the elastic constants were found to pass through minima as a function of temperature. The results were quantitavely explained by a model which assumes simple forms of the molecular excitation spectrum. An alternative interpretation, though being only qualitative, postulates a freezing of the CN molecules into a glass-like phase.

Modulated magnetic structures of ErPb3, HoPb3, ErTl3 and HoTl3

Neutron diffraction experiments have been carried out on the magnetically ordered phases of ErPb3, HoPb3, ErTl3 and HoTl3. The magnetic moments were found to be sinusoidally modulated with a propagation vector of (0, 0.2, 0.5) for the Pb-compounds and (0.38, 0.38, 0.16) for the Tl-compounds.

Superconductivity and magnetism in Rb0.8Fe1.6Se2under pressure

High-pressure magnetization, structural and 57Fe M\"ossbauer studies were performed on superconducting Rb0.8Fe1.6Se2.0 with Tc = 32.4 K. The superconducting transition temperature gradually decreases on increasing pressure up to 5.0 GPa followed by a marked step-like suppression of superconductivity near 6 GPa. No structural phase transition in the Fe vacancy-ordered superstructure is observed in synchrotron XRD studies up to 15.6 GPa, while the M\"ossbauer spectra above 5 GPa reveal the appearance of a new paramagnetic phase and significant changes in the magnetic and electronic properties of the dominant antiferromagnetic phase, coinciding with the disappearance of superconductivity. Thes…

Elastic and quasielastic neutron scattering studies in KBr:KCN mixed crystals

Neutron scattering studies in (KBr)1–x(KCN)x mixed crystals are presented utilizing powder diffraction, single crystal diffraction and time-of-flight techniques. Forx&gt;0.6 (KBr)1–x(KCN)x crystals exhibit ferroelastic and ferroelectric low-temperature phases. Crystals withx&lt;0.6 undergo transitions into an orientational glass state. Here we present a detailed phase diagram including new results for x=0.85 and x=0.65. For the latter system a stable rhombohedral low-temperature phase has been detected where the orientational disorder of the plastic phase is only partly removed and quadrupolar relaxations between three body diagonals are still possible. From the powder diffraction experimen…

Neutron diffraction study of the heavy fermion superconductors UM2Al3(M=Pd, Ni)

An elastic neutron scattering study was performed on the new superconducting heavy fermion systems UPd2Al3 and UNi2Al3. The neutron diffraction patterns reveal unambiguously long range antiferromagnetic order in UPd2Al3 with an ordered magnetic momentμ U = (0.85±0.03)μ B , which coexists with the superconducting state. This is by far the largestμ U value observed for any heavy fermion superconductor. For UNi2Al3, no long-range magnetic order could be observed for temperaturesT≧1.5 K, yielding an upper limit of the ordered moment of 0.2μ B .

Alloying-induced transition from local-moment to itinerant heavy fermion magnetism in Ce(Cu1−xNix)2Ge2

Abstract A monotonous increase of the Kondo temperature in Ce(Cu1−xNix)2Ge2 from 7 (x = 0) to 30 K (x = 1) is accompanied by drastic changes of ground state properties: for x⩽0.2, a modulated magnetic structure (q01 = (0.28, 0.28, 0.54)) involving Kondo-reduced local Ce moments ( μ s = 0.74μ B Ce for x = 0) forms below TN1(x). TN1 = 4. 1 K for CeCu2Ge2 is strongly depressed upon increasing x. At x ≲ 0.2, a different modulation develops below TN2(x) which becomes maximum (≃4 K) for x = 0.5. Since this is characterized by a very small value of q02 (=(0, 0, 0.13) at x = 0.5) and a gradually decreasing ordered moment (reaching μs ≲ 0.2μB/Ce for x ⩾0.65), we ascribe it to “heavy fermion band mag…

Direct observation of the quasiparticle relaxation in YBa2Cu3O7

Abstract The real and imaginary parts of the optical conductivity ( σ 1 + iσ 2 ) in the superconducting state of YBa 2 Cu 3 O 7−δ thin films have been obtained by submillimeter spectroscopy for frequencies from 3 to 35 cm −1 . The quasiparticle relaxation can be directly observed in this frequency range. A Drude-type analysis allows to extract the temperature dependence of the scattering rate. The collapse of the relaxation rates provides clear experimental evidence that the spin fluctuations become gapped below T C .

Polar relaxation mode in pure and iron-doped barium titanate

A dielectric relaxation peak is reported in ${\mathrm{BaTiO}}_{3}$ and in ${\mathrm{BaTi}}_{1\mathrm{\ensuremath{-}}\mathrm{x}}$${\mathrm{Fe}}_{\mathrm{x}}$${\mathrm{O}}_{3}$. It is nearly monodispersive, centered in the ${10}^{8}$-Hz range, and slowest at the transition temperature ${T}_{c}$\ensuremath{\simeq}413 K from the cubic to the tetragonal phase. Iron doping lowers ${T}_{c}$ and slows down this relaxation mode.

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Soft modes and mode splitting in paramagnetic TbP§

In contrast to spin-only systems the paramagnetic phases of systems with crystal field split ground multiplets exhibit magnetic excitations of finite energy. In the presence of a magnetic exchange coupling the excitons will propagate through the lattice. A measurement of the dispersion allows in principle an insight into the exchange interaction, which is of fundamental importance for the understanding of the magnetic phenomena. Unfortunately the evolution of the dispersion at low temperatures is in most cases interrupted by the onset of magnetic order due to an alignment of the magnetic moments of the crystal field ground state. A noticeable dispersion of well-defined excitons is only expe…

Nonresonant Spectral Hole Burning in the Slow Dielectric Response of Supercooled Liquids

Large-amplitude, low-frequency electric fields can be used to burn spectral holes in the dielectric response of supercooled propylene carbonate and glycerol. This ability to selectively modify the dielectric response establishes that the non-Debye behavior results from a distribution of relaxation times. Refilling of the spectral hole was consistent with a single recovery time that coincided with the peak in the distribution. Moreover, refilling occurred without significant broadening, which indicates negligible direct exchange between the degrees of freedom that responded to the field. Nonresonant spectral hole burning facilitates direct investigation of the intrinsic response of systems t…

Singlet ground state magnetism: II. magnetic excitons in paramagnetic TbP

The magneticΓ 1 –Γ 4 exciton of the singlet ground state system TbP has been studied by inelastic neutron scattering above the antiferromagnetic ordering temperature. Considerable dispersion and a pronounced splitting was found in the [100] and [110] directions. Both the band width and the splitting increased rapidly as the transition temperature was approached in accordance with the predictions of the RPA-theory. The dispersion is analysed in terms of a phenomenological model using interactions up to the fourth nearest neighbour.

Universal relationship between the penetration depth and the normal-state conductivity in YBaCuO

The absolute values of the conductivity in the normal state sigma_n and of the low temperature penetration depths lambda(0) were measured for a number of different samples of the YBaCuO family. We found a striking correlation between sigma_n and 1/lambda^2, regardless of doping, oxygen reduction or defects, thus providing a simple method to predict the superconducting penetration depth and to have an estimate of the sample quality by measuring the normal-state conductivity.

Frequency-dependent relaxation rate in superconductingYBa2Cu3O6+δ

The submillimeter-wave $3 {\mathrm{cm}}^{\ensuremath{-}1}l\ensuremath{\nu}l40 {\mathrm{cm}}^{\ensuremath{-}1}$ complex conductivity of the reduced ${\mathrm{YBa}}_{2}{\mathrm{Cu}}_{3}{\mathrm{O}}_{6+\ensuremath{\delta}}$ film ${(T}_{C}=56.5 \mathrm{K})$ was investigated for temperatures $4 \mathrm{K}lTl300 \mathrm{K}$ and compared to the properties of the same film in the optimally doped state. The frequency dependence of the effective quasiparticle scattering rate $1/{\ensuremath{\tau}}^{*}(\ensuremath{\nu})$ was extracted from the spectra. $1/{\ensuremath{\tau}}^{*}$ is shown to be frequency independent at low frequencies and high temperatures. A gradual change to $1/{\ensuremath{\tau}}^{…

Dipolar and Quadrupolar Freezing in(KBr)1−x(KCN)x

Dipolar and quadrupolar susceptibility measurements are reported for the molecular glass system ${(\mathrm{KBr})}_{1\ensuremath{-}x}{(\mathrm{KCN})}_{x}$ covering a wide range of frequencies. The results allow a direct comparison of the dipolar and quadrupolar anomalies and demonstrate unambiguously that the freezing in of the dipolar and quadrupolar degrees of freedom occurs at different temperatures.

The analysis of dielectric relaxation phenomena with the inverse Fourier transformation

Abstract A method to determine the distribution of relaxation times directly from dielectric loss spectra is presented. The method is based upon a deconvolution procedure: the Fourier transform of the loss factor is divided by sech( π 2 f ) and then, via an inverse Fourier transformation, transformed into the time domain. Limitations and possible improvements of the method are discussed. It is shown that the present method is able to reveal local relaxation processes not perceptible in the loss factor spectrum. With stimulated noise-free data, the resolution of the method is one third of a decade on a logarithmic relaxation timescale.

Hopping conductivity in NiO thin films

Structural relaxation in a molten salt probed by time-dependent dc conductivity measurements

Abstract Time-dependent dc conductivity was measured after cooling steps of about 2 K in the glass transformation range of 2Ca(NO 3 ) 2 -3RbNO 3 . The shape and time scale of the structural relaxation function was thus monitored for times 60 s t 6 s. The time scale could be compared with results from scanning calorimetry measurements and good agreement was found. From the heat capacity data and from the solid state conductivity the expected liquid state conductivity relaxation time was calculated using several models. The good compatibility of these calculations with the experimental results provides evidence that near the calorimetric glass transition the mobile ions perform concerted moti…

Magnetic order in the heavy fermion system Ce(Cu1−xNix)2Ge2

Abstract The magnetic phase diagram of the heavy fermion (HF) systems Ce(Cu 1−x Ni x ) 2 Ge 2 is discussed utilizing results of transport, thermodynamic and neutron-scattering measurements. While the Kondo temperature increases monotonically with x, a complex x-dependence is found for the Neel temperature, associated with a transition from local-moment to itinerant HF magnetism.

Phase separation in superconducting and antiferromagneticRb0.8Fe1.6Se2probed by Mössbauer spectroscopy

${}^{57}$Fe-M\"ossbauer studies of superconducting Rb${}_{0.8}$Fe${}_{1.6}$Se${}_{2.0}$ with ${T}_{C}$ $=$ 32.4 K were performed on single-crystalline and polycrystalline samples in the temperature range 4.2--295 K. They reveal the presence of 88% magnetic and 12% nonmagnetic Fe${}^{2+}$ species with the same polarization dependence of their hyperfine spectra. The magnetic species are attributed to the 16$i$ sites of the $\sqrt{5}\ifmmode\times\else\texttimes\fi{}\sqrt{5}\ifmmode\times\else\texttimes\fi{}1$ superstructure and the nonmagnetic Fe species to a nanosized phase observed in recent structural studies of superconducting K${}_{x}$Fe${}_{2\ensuremath{-}}$${}_{y}$Se${}_{2}$ systems ra…

X-ray diffraction on (KBr)1−x(KCN)xmixed crystals

The molecular glass state in KBr1-x (CN)x

Structural and dynamic properties of the molecular glass KBr1-x (CN)X are reported. The low temperature state can be characterized as an averaged crystal, where clusters of correlated frozen-in CN- ions yield a distribution of frozen-in lattice strains which destroy the rigorous center-of-mass periodicty of the high temperature phase. The freezing process measured via cusps in the dipolar and quadrupolar susceptibilities is a relaxional phenomenon and depends sensitively on the timescale of the experiment.

Pressure effect on superconductivity in FeSe0.5Te0.5

Due to the simple layered structure, isostructural FeSe and FeSe0.5Te0.5 are clue compounds for understanding the principal mechanisms of superconductivity in the family of Fe-based superconductors. High-pressure magnetic, structural and Mossbauer studies have been performed on single-crystalline samples of superconducting FeSe0.5Te0.5 with Tc = 13.5 K. Susceptibility data have revealed a strong increase of Tc up to 19.5 K for pressures up to 1.3 GPa, followed by a plateau in the Tc(p) dependence up to 5.0 GPa. Further pressure increase leads to a disappearance of the superconducting state around 7.0 GPa. X-ray diffraction and Mossbauer studies explain this fact by a tetragonal-to-hexagonal…

Correlated barrier hopping in NiO films

The ac conduction in NiO films has been investigated in the frequency range 10 Hz < v < 10^9 Hz and at temperatures between 10 and 300 K. The frequency and the temperature dependence of the electrical conductivity can be consistently explained within a model developed for the mechanism of charge transfer in amorphous semiconductors which proposes that charge carriers hop over potential barriers between defect sites, the height of the barriers being correlated with the intersite separation.

Singlet ground state magnetism: III. magnetic excitons in antiferromagnetic TbP

The dispersion of the lowest magnetic excitations of the singlet ground state system TbP has been studied in the antiferromagnetic phase by inelastic neutron scattering. The magnetic exchange interaction and the magnetic and the rhombohedral molecular fields have been determined.

Optical conductivity inYBa2Cu3O7−δthin films

The real and imaginary parts of the optical conductivity ${\ensuremath{\sigma}}_{1}+i{\ensuremath{\sigma}}_{2}$ of partly untwinned ${\mathrm{YBa}}_{2}{\mathrm{Cu}}_{3}{\mathrm{O}}_{7\ensuremath{-}\ensuremath{\delta}}$ thin films were measured by submillimeter spectroscopy for frequencies from 100 GHz to 1 THz. The frequency dependence of the conductivity below ${T}_{C}$ can be described by a narrow Drude-like peak with strongly temperature-dependent relaxation rates. ${\ensuremath{\sigma}}_{1}(\ensuremath{\nu})$ does not extrapolate to the universal d-wave value at 0 K. Impurity scattering significantly different to the unitary limit has to be assumed to achieve agreement with recent theor…

Relaxation times at the rate-dependent glass transition

The structural relaxation time near the cooling rate dependent glass transition is determined self-consistently within the Moynihan-Narayanaswami formalism. In order to illustrate the method we analyze scanning calorimetry data from amorphous calcium-rubidium nitrate. A characteristic time scale of about 250 s is obtained at the conventionally defined glass transition. The occurrence of decoupled, faster relaxation modes is briefly discussed.

Dielectric properties of (KBr)1-x (KCN)x

The temperature dependence of the dielectric constant of (KBr)1−x (KCN) x was measured at frequencies of 87.5 Hz, 1, 10 and 100 kHz for concentrations ofx=0, 0.01, 0.04, 0.14, 0.25, and 0.50. Both the real and the imaginary part showed maxima at characteristic temperatures which depend on the measuring frequency and the concentration. The results are analogous to the behaviour of the magnetic susceptibility in spin glasses and support the existence of an orientational glass state.

Proton glass behavior and hopping conductivity in solid solutions of antiferroelectric betaine phosphate and ferroelectric betaine phosphite.

Measurements of the dielectric permittivity are reported for solid solutions of antiferroelectric betaine phosphate and ferroelectric betaine phosphite at frequencies 10 −2 Hz T c the dielectric response is dominated by ac and dc conduction. The 40% sample exhibits pure relational behavior indicative of a transition into an orientational glass state

Relaxational dynamics at the class transition in orientational and canonical glasses investigated by dielectric spectroscopy

Abstract Measurements of the dielectric permittivity are reported for the canonical glass glycerol and for solid solutions of ferroelectric betaine phosphite and ferroelectric betaine phosphate, which can be viewed as protype systems of orientational glasses. In this latter system long range dipolar order is suppressed by the competing ferroelectric and antiferroelectric interactions and the dipolar moments freeze-in devoid of long range order. In both systems the relaxation dynamics is studied for frequencies 10−2Hz≤ν≤106Hz, close to the glass transition temperature. The relaxation dynamics is characterized according to Angell's classification scheme of strong and fragile glass-formers.

Pressure effect on superconductivity in FeSe0.5Te0.5

Due to the simple layered structure, isostructural FeSe and FeSe0.5Te0.5 are clue compounds for understanding the principal mechanisms of superconductivity in the family of Fe-based superconductors. High-pressure magnetic, structural and M\"ossbauer studies have been performed on single-crystalline samples of superconducting FeSe0.5Te0.5 with Tc = 13.5 K. Susceptibility data have revealed a strong increase of Tc up to 19.5 K for pressures up to 1.3 GPa, followed by a plateau in the Tc(p) dependence up to 5.0 GPa. Further pressure increase leads to a disappearance of the superconducting state around 7.0 GPa. X-ray diffraction and M\"ossbauer studies explain this fact by a tetragonal-to-hexag…

Statics and Dynamics of a Glassy Crystal: A NMR- and Neutron Scattering Investigation of (NaCl) 0.35 (NaCN) 0.65

The statics and the dynamics of the glass transition in (NaCl)0.35(NaCN)0.65 have been investigated by inelastic neutron scattering and are directly compared to NMR results. Insight into the relaxation dynamics is gained via the temperature dependence of the transverse acoustic phonon modes and via the spin relaxation time T1. The statics of the system is reflected by the growth of a central peak and by the distribution of electric-field gradients. Both quantities are directly related to the glass order parameter. The temperature dependence of the order parameter provides experimental evidence that in NaCl:NaCN mixed crystals the glass transition is dominated by random fields rather than by…

Neutron diffraction experiments on UCu4+xAl8−x

Abstract Neutron diffraction experiments are reported on UCu4+xAl8−x for concentrations 0.1≤ x ≤1.9 and temperatures 1.6 K≤T≤300 K. For x ≤ 1 these compounds undergo antiferromagnetic phase transitions into a collinear AF I-type structure. with the magnetic moments aligned along the tetragonal c-axis and alternating order within the a−b planes. With increasing concentration the ordering temperatures decrease and moment compensation due to a Kondo-type interaction develops for x>1.

Phases and phase transitions in the mixed molecular system (NaCN)1x(KCN)x

The phase diagram of (NaCN)1−x(KCN)x was examined by neutron powder diffraction in the temperature range 5K ≦T≦300 K. Several non-cubic low-temperature phases were identified for concentrationsx<xc1=0.15 andx≧xc2=0.89. Lattice parameters and ferroelastic deformations were determined from the observed powder patterns. The phase transformations were characterized following the temperature dependence of the appropriate order parameters.

Inelastic neutron scattering study of the rotational excitations in(KBr)1−x(KCN)xin the paraelastic and structural glass state

The coupled rotational-translational excitations in ${(\mathrm{KBr})}_{1\ensuremath{-}x}{(\mathrm{KCN})}_{x}$ were studied by inelastic neutron scattering for concentrations $0.008\ensuremath{\le}x\ensuremath{\le}0.20$. We followed the ${A}_{1g}\ensuremath{-}{T}_{2g}$ tunneling transition and the ${A}_{1g}\ensuremath{-}{E}_{g}$ librational excitation through the transition from the paraelastic to the structural glass state. We found that these two excitations and their coupling to the lattice strains exhibit a very different temperature dependence in the glass state. While the tunneling transition, which triggers reorientations of the ${\mathrm{CN}}^{\ensuremath{-}}$ ions, shows a drastic r…

Singlet-groundstate magnetism in TbP

Elastic neutron scattering and magnetic susceptibility data are reported for temperatures around the Neel-point,TN=7.3 K, and for zero magnetic field. AboveTN, the temperature dependence of the magnetic central peak intensity can adequately be described within the RPA assuming isotropic exchange between nearest and next-nearest neighbours as the only parameters. This two-parameter model is quantitatively confirmed by the susceptibility data. AtTN, magnetic Bragg-intensities arise almost discontinuously (reaching 70% of the saturation within 0.1 K) accompanied by thermal hysteresis. For all temperatures belowTN the sublattice magnetic moment is explained by solutions of meanfield equations, …

Phases and phase transitions of (NaCl)1?x(NaCN)x

(NaCl)1−x(NaCN)x mixed crystals with CN-concentrationsx of 0.87, 0.76, 0.71 and 0.65 have been investigated by X-ray powder diffraction. Apart from the cubic room temperature phase, a rhombohedral and an orthorhombic phase have been identified. In addition a glass state has been observed which is characterized by a strong broadening of the cubic powder lines. The phase diagram shows a wide coexistence gap between the non-cubic phases and the glass state.

Reorientations and phase transitions in (Kr)1-x(CH4-nDn)x

The condensed isotopic modifications of methane, CH4, CH2D2, and CD4 and their solutions with Kr were investigated using dielectric techniques. The polarizabilities were computed from the permittivities of the pure liquids. Phase diagrams of methane-krypton alloys were deduced in the liquid-solid coexistence region and for the low temperature phases (T&lt;30 K). From the Curielaws, which described the permittivities of the (Kr)1-x(CH2D2)x mixed crystals, the permanent dioole moment of CH2D2 is calculated to be 4 mD. In the octopolar ordered phases of the solid solutions the effective dipole moments are enhanced significantly.

High frequency resistivity in La2-xSrxCu1-yCoyO4 ceramics

Resitivity measurements have been performed in La:Sr:Cu:Co:O ceramics in a frequency range from 5Hz – 10 9 Hz. A strongly frequency dependent resistance has been observed in La 2 CUO 4 which we interpret in terms of a smooth dielectric to metal transition due to localization effects.

Neutron powder diffraction study in the mixed molecular system (NaCN)1−x(KCN)x

A detailed structural analysis of (NaCN${)}_{1\mathrm{\ensuremath{-}}\mathrm{x}}$(KCN${)}_{\mathrm{x}}$ mixed crystals with x=0.02, 0.19, and 0.95 was performed by neutron powder diffraction. The structural parameters of the cubic phases were refined, applying a model of preferred orientations. Different noncubic low-temperature phases were observed for x=0.02 and 0.95. For x=0.02 the antiferroelectric ordering of ${\mathrm{CN}}^{\mathrm{\ensuremath{-}}}$ dipoles at low temperatures is accompanied by significant alkali-alkali and alkali-${\mathrm{CN}}^{\mathrm{\ensuremath{-}}}$ sublattice shifts. Structural data are presented together with previous results for mixed crystals with x=0.59 and…

Dielectric study of supercooled triphenylphosphite and butyronitrile: Comparison with a mesoscopic model

Abstract Dielectric relaxation has been studied in the supercooled liquids triphenylphosphite (TPP) and butyrontrile (BN). BN is relatively strong according to Angell's classification and can be characterized by a fragility index m = 47. TPP, on the other hand, appears to be the most fragile non-polymeric liquid studied so far (m = 160). The dielectric response of the two glass-formers exhibits different degrees of non-exponentiality which is analyzed in terms of a mesoscopic model of dynamically correlated domains. The relation of this model to the strong versus fragile liquid classification scheme is discussed.

Magnetic order in UCu4+xAl8−x

Abstract A neutron diffraction study has been performed on UCu4+xAl8−x. The compound was chosen as an example of a uranium-based system, which goes from a magnetically ordered state to a pure heavy-fermion state. In the range x = 0.25–1, UCu4+xAl8−x orders in a simple collinear antiferromagnetic structure. With increasing concentration of Cu, the ordering temperature decreases and moment compensation develops due to the increasing hybridization of the 5f electrons.

Dielectric investigations of pure and mixed fluorocarbons in their condensed phases

We review recent work and present new results on the liquid and solid fluocarbons CMF3 with M = H, F, Cl, Br, CH3, and CF3. The pure compounds as well as several series of binary mixtures were investigated using dielectric measurements. The permittivities of the non-hydrogenatcd non-polar and polar liquids could be described using the Clausius-Mosotti and the Onsager equation, respectively. In CHF3 and C2H3F3 hydrogen bridging leads to deviations from this simple behavior. The trends in the miscibility of four series of fluorocarbon mixtures are in qualitative accord with regular solution theory. The geometrical shapes of the compounds dominate the degrees of order below their melting point…

Mössbauer gamma-ray diffraction from the molecular crystal KCN

Abstract Mossbauer gamma-ray diffraction was applied to separate the elastic and inelastic scattering intensities from the (200), (400) and (600) Bragg reflections of KCN. The energy resolution of our experiment was 60 neV. The Debye-Waller factor extracted from the elastic data and the thermal diffuse inelastic data both increase towards phase transition, theoretically a logarithmic singularity was predicted.

A neutron diffraction study of the glass transition in (KBr)0.47(KCN)0.53

Abstract The molecular crystal (KBr) 0.47 (KCN) 0.53 has been investigated by elastic neutron diffraction at the transition from the paraelastic to the orientational glass state. The freezing temperature is characterized by the onset of a momentum transfer dependent broadening of the diffraction lines indicating the transition from a crystalline to an amorphous state.

Anomalous diffraction profiles of alkali-halide-alkali-cyanide mixed crystals.

The x-ray diffraction profiles of four mixed alkali halides-alkali cyanides have been studied. At the threshold concentration where the systems change over from ferroelastic ordering to the glass state, the profiles are highly unusual. The diffracted intensity of transverse scans along the cubic axes follows $I\ensuremath{\sim}\mathrm{exp}(\ensuremath{-}\ensuremath{\alpha}|\ensuremath{\xi}|)$, where $\ensuremath{\xi}$ is the reduced wave vector, measured from the line center.