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…

Positive Muons as Local Probes in Paramagnetic Rare Earth Systems

In recent years a new research method has been developed in solid state physics which is based on the asymmetry of muon decay1. A positive muon at rest decays after a mean lifetime of 2.2 μsec into a positron and two neutrinos, the positron being emitted preferentially in the direction of the muon spin. Hence if spin polarized muons are implanted in a solid, the time evolution of the muon spin polarization can be determined by a measurement of the angular distribution of the positrons. In an external magnetic field transverse to the initial spin direction of the muon one can study the muon spin precession frequency, which is determined by the actual field at the muon, and τ2-relaxation effe…

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.

Crystal Fields in Pr-Hydrides

Inelastic neutron scattering was used to determine the crystal field splittings of PrD2 and PrD2.5. For the PrD2 crystal field at the Pr-site is cubic and can be explained by a negative charge of the hydrogen. The splitting observed for PrD2.5 can be described assuming a well defined short range order caused by a mer-configuration of the half filled octahedral hydrogen sites leading to an orthorhombic crystal field. The structure and the paramagnetic susceptibility of the Pr-hydrides are discussed on this basis.

X-ray-diffraction study of the crystal structures and orientational glass state ofAr1−x(N2)xsolid solutions

Solid solutions of ${\mathrm{Ar}}_{1\mathrm{\ensuremath{-}}\mathit{x}}$(${\mathrm{N}}_{2}$${)}_{\mathit{x}}$ have been investigated by x-ray powder diffraction in the range 0.5x1.0, 8T60 K, and under hydrostatic pressures up to 2200 bars. The structural hcp-cubic (Pa3) phase transition is identified as a martensitic transformation with a wide transformation hysteresis. For x0.8 and T30 K the solid solutions show the orientational glass state, which is characterized by a superposition of inhomogeneous and homogeneous lattice strains. The inhomogeneous component is described by the random-field model. The homogeneous component corresponds to an orthorhombic distortion of the hcp lattice. Two …

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.

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.

Muon Knight shift studies of the valence transition in Ce0�74Th0�26

Crystal Electric Fields in Rare-Earth Al2 Compounds

Neutron time-of-flight measurements have been performed on REAl2 compounds (RE = Pr, Ho, Er, Tm) in the paramagnetic region. Resolved crystal field transitions are observed in ErAl2 and TmAl2. We deduce crystal field parameters (x = 0.16, W = -0.030 meV) and (x = -0.28, W = +0.040 meV) for ErAl2 and TmAl2 respectively.

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

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.

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…

A neutron scattering study of the magnetic properties of PrSn3

The intermetallic compound PrSn3 has been studied by elastic and inelastic neutron scattering. The paramagnetic phase shows overdamped crystal field excitations and an anisotropic distribution of the diffuse magnetic intensity. The dispersion relation of the excitations of the antiferromagnetic phase has been determined. The results are analyzed in terms of an anisotropic exchange coupling.

Crystal field splitting of some rare earth intermetallic compounds with Cu3Au structure

Inelastic neutron scattering studies were performed in the paramagnetic phases of several rare earth compounds that crystallize in the cubic Cu3Au structure: ErPb3, ErTl3, ErIn3, HoPb3, HoTl3, HoIn3, PrSn3, PrPb3, PrTl3, PrIn3, CeIn3, La1−c Pr c Tl3, and Pr(In0.5Tl0.5)3. The energies, widths and intensities of the crystal field excitations are determined and discussed in terms of interactions between the rare earth ions. Variations of the crystal field parameters are observed across the series.

Crystal Field Excitations in CeAgl−xInx Compounds

The substitution of the monovalent Ag for the trivalent In in LaAgl−xInx and CeAgl−xInx offers the possibility of influencing the conduction electron system in these compounds. The strong dependence of the spin susceptibility of La-systems on the In-concentration1 was interpreted by band calculations which suggest that the Fermi level is pushed into a region of a high 5d-eg-band density of states2. Furthermore, CeAgl−xInx is one of the rare 4f systems where a structural phase transition (from cubic to tetragonal) occurs prior to magnetic ordering. The ferromagnetic Curie temperature TC is roughly independent of x whereas the structural transition temperature Ts rises from 15 K for CeAg to a…

Martensitic phase transformation cubic-orthorhombic of NaCN and (NaCN)0.98 (KCN)0.02

The ferroelastic cubic-orthorhombic transition of single crystals NaCN and (NaCN)0.98 (KCN)0.02 has been studied by x-ray diffraction. The domain configuration obtained is consistent with the Wechsler, Lieberman, Read-model for martensitic transformations.

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.

LaAg x In1?x

The phonon dispersion of LaAg x In1−x (x=1, 0.89, 0.8) has been studied by inelastic neutron scattering in the cubic high temperature phase. A soft mode behaviour was observed at theM-point. The doubling and the cubic to tetragonal deformation of the elementary cell was observed through the phase transition. The measurements of the elastic constants were extended to 450 K and their magnetic field dependence was investigated.

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

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.

Effects of pressure and of thermal history on the structural phase transition of KCN

The cubic-noncubic structural phase transition of a KCN single crystal is studied as a function of thermal history and of hydrostatic pressure up to 2 kbar. The standard sequence of phases is cubic-monoclinic-orthorhombic on cooling and orthorhombic-cubic on heating. The monoclinic phase is also absent in first cooling runs at low pressures (p≦250 bar). The width of the monoclinic field inp, T phase diagram is increased in second cooling runs. The effects are discussed in terms of a martensitic transformation behavior and random strain fields.

Ellipsometric study of the physisorption of benzene on graphite

The optical thickness of benzene on the (001) surface of a graphite single crystal has been studied by ellipsometry. Ellipsometric adsorption isotherms have been measured in the temperature range from 180 to 290 K. The maximum thickness of the adsorbed benzene film is constant in this temperature range and compares favourably with the value expected for one monolayer of molecules lying flat on the surface.

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.

Oxide growth and tunneling characteristics of Sn-SnO x -Sn junctions

Sn—SnOx—Sn tunneling junctions were prepared by thermal oxidation of vacuum deposited Sn-films. The thickness growth of the oxide was followed by ellipsometric measurements. From logarithmic conductivity measurements the barrier heights were determined. The tunneling characteristic could be well described by the two-band-tunneling model using a value of 0.14 for the ratio of the effective masses in the oxide and the metal.

Ferroelastic phase transitions of alkali halide-alkali cyanide mixed crystals

Abstract The alkali cyanides and their CN-rich mixtures with alkali halides are proper ferroelastics with transitions from the cubic high temperature phase into the various non-cubic low temperature phases. As the CN concentration is reduced, the transformations temperature decreases and eventually the ferroelastic low temperature state is suppresse in favour of a glass-like state. The structural and elastic properties of these compounds are discussed with a special emphasis on the martensitic aspect of the transitions.

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.

Sequential Freezing of Quadrupolar and Dipolar Order in (KBr)1-x(KCN)xGlassesa

Random-strain-field effects on the low-temperature state of KCN

Random strain fields have been introduced into samples of KCN by pressing pellets from powder and by thermal cycling. X-ray diffractograms show that the low-temperature structure depends strongly on the sample history. In some cycles the noncubic low-temperature phases have been suppressed in mesoscopic surface regions of the samples and the quadrupolar-glass state formed instead.

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.

Neutron scattering and crystal fields in Pr-hydrides

The crystal field splittings of PrD2 and PrD2.5 have been determined by inelastic neutron scattering. While for PrD2 the crystal field experienced by the majority of Pr-ions is cubic, it is shown that in PrD2.5 the occupation of the octahedral interstitials occurs not in a statistical but rather in a well defined way which leads to an orthorhombic crystal field at the Pr-site.

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.

Muon Knight-shift measurements in CeSn3and some isostructural rare-earth compounds

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>0.6 (KBr)1–x(KCN)x crystals exhibit ferroelastic and ferroelectric low-temperature phases. Crystals withx<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…

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…

X-ray diffraction study of CF3Cl monolayers adsorbed on graphite (001)

X-ray diffraction experiments have been performed on mono- and submonolayers of CF3Cl physisorbed on the (001) surfaces of exfoliated graphite. Five quasi-twodimensional solid phases including the commensurate 2×2 phase, an electrically ordered phase and a disordered incommensurate phase have been observed. A phase diagram is proposed and the various phase transitions are discussed.

The difference of crystal fields in ErAl2 and La0.9Er0.1Al2

Abstract Inelastic neutron scattering experiments have been carried out on polycrystalline ErAl2 and on the related pseudobinary compound La0.9Er0.1Al2 in the paramagnetic phase. For ErAl2 the parameters of the cubic crystal field could uniquely be determined as x=+0.16 and W=−0.030 meV. The results on the dilute sample are different from this and are thought to be due effective charges of Er and La being not equivalent.

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…

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.

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.

Shear elasticity of mixed cyanide orientational glass

Four mixed crystals of KBr:KCN and NaCN:KCN, complemented by KCN, have been investigated by torque-shear measurements. The real and imaginary parts of the shear compliance ${\mathit{s}}_{44}$ at a measuring frequency of 2 Hz have been determined. Zero-field-cooling--field-cooling--remanent-shear-strain cycles have been performed. For (KBr${)}_{0.47}$(KCN${)}_{0.53}$ the creep after zero-field cooling and the elastic aftereffect after field cooling have been followed within a time window from 0.1 to ${10}^{4}$ s. Results on the nonlinear part of the shear compliance have been obtained. It is shown that the field-cooled strain represents the static limit of the elastic response. The results a…

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

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.

Field-cooling experiments on the quadrupolar-glass state of (KBr)0.47(KCN)0.53

The shear strain of a mixed cyanide crystal has been measured under field-cooling conditions. The time decay after field removal follows a Kohlrausch-Williams-Watts law. The results are analogous to spin glasses, except that residual permanent strains can be frozen-in.

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.

Ellipsometric thickness and coverage of physisorbed layers of Xe, Kr, Ar and N2 on graphite

Multilayer isotherms of Xe, Kr, Ar and N2 physisorbed on graphite (001) have been studied by ellipsometry. It is shown that the model of Dignam and Fedyk provides an excellent basis for the interpretation of the ellipsometric thickness in terms of the coverage and the polarizability of the admolecules. For N2 conclusions concerning the orientation of the molecule are drawn.

Two-dimensional electrical ordering in physisorbed monolayers

Abstract Monolayers of polar molecules CF3H, CF3Cl and CF2Cl2 have been physisorbed on the graphite (001) surface and studied by X-ray diffraction and dielectric measurements. The temperature-coverage phase diagrams of the quasitwodimensional crystalline phases are presented. The structures of the paraelectric and the electrically ordered phases have been determined. The phase transitions are discussed.

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…

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.

Crystal Fields in PrX3 (X=In, Tl, Pb, Sn) Intermetallic Compounds with Cu3Au Structure

We have determined the crystal field splittings of Pr3+ in PrIn3, PrTl3, PrPb3, and PrSn3 by inelastic neutron scattering. The values of the deduced crystal field parameters are found to depend strongly on the constituent X, though all systems have nonmagnetic ground-states. The line widths in the different systems are compared.

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.

Polymorphism and the glasslike state of cyanide mixed crystals: A mesoscopic problem.

The martensitic aspect of the structural phase transitions of the alkali cyanides and their solid solutions with the alkali halides is discussed. It is suggested that the polymorphism is intimately connected with the problem of mesoscopic transformation strains. At intermediate CN concentrations a competition between glasslike inhomogeneous strains, modulated strains, and ferroelastic strains is observed.