ESR of Gd-impurities in the heavy fermion compounds CeCu2Si2 and CeAl3

The heavy fermion systems CeCu₂Si₂ and CeAl₃ are characterized by a huge quasiparticle density of states responsible for the large electronic specific heat. The observation of a Gd³⁺ electron spin resonance (ESR) in single crystals CeCu₂Si₂ and in polycrystalline CeAl₃ clearly demonstrates the local character of these quasiparticles. Nevertheless, the Gd-spin relaxation shows remarkable anomalies with respect to the isostructural compounds LaCu₂Si₂ and LaAl₃: Probably via RKKY coupling, Ce 4f-spin fluctuations give rise to an enhanced Gd-spin relaxation resulting in an unusual non-linear thermal broadening around the Kondo temperature. From this we obtain information about the temperature dependence of the Ce 4f-spin correlation time.     

EPR study of exchange interactions in the nonmagnetic Kondo system La1−x CexCu6

The EPR of paramagnetic impurities Gd³⁺ and Mn²⁺ was studied in nonmagnetic Kondo system La_1−x Ce_xCu₆ containing in the 1.6–200 K range. The exchange interaction parameters of gadolinium and manganese ions with conduction electrons, of cerium ions with conduction electrons and with one another, the Kondo temperature of cerium ions, and the temperature behavior of cerium-ion spin-fluctuation rate have been determined. A pseudogap in the density of states at the Fermi level has been detected in the CeCu₆ regular system, which is apparently due to s-f hybridization. This pseudogap can be destroyed by introducing an aluminum impurity, which induces strong conduction-electron scattering. It was also found that RKKY interaction among manganese ions in CeCu_6−y Mn_y is considerably stronger than it is in LaCu_6−y Mn_y, which implies enhancement of nonlocal spin susceptibility due to an f band contribution to conduction-electron states. Fiz. Tverd. Tela (St. Petersburg) 40, 593–599 (April 1998)     

On the theory of superconductivity in Kondo lattice systems

An attempt is made to explain the occurrence of superconductivity in Kondo lattice systems with special reference to CeCu₂Si₂. Starting point is the Fermi liquid approach. It is generalized from a Kondo impurity to the Kondo lattice by means of the Korringa-Kohn-Rostocker method. From it a hybridization model is derived and discussed in detail. Two electron-phonon mechanisms are investigated which appear in Kondo lattices. One results from the additional phase shifts caused by the Kondo ions while the other is responsible for the so-called Kondo volume collapse. It is shown that the latter is sufficiently strong in order to explain why CeCu₂Si₂ is a superconductor while LaCu₂Si₂ is not. An estimate for the superconducting transition temperatureT _c produces the right order of magnitude.     

Transport properties and point-contact spectra of RECu6 with RE=La,Ce and Pr

Measurements of the current-voltage characteristics on point-contacts, of the thermopower and the thermal conductivity between 1.3 and 300 K and of the electrical resistivity between 4.2 and 900 K of polycrystalline samples of ReCu₆ (RE=La, Ce, Pr, Gd) are presented. The anomalies of the heavy fermion system CeCu₆ are strong compared to the other systems, but the properties of LaCu₆ and PrCu₆ are also unusual, possibly caused by the complicated crystal structure and, for PrCu₆, by crystal field effects.     

Structural properties and band structure of heavy fermion systems: CeCu2Si2 and LaCu2Si2

The structure of CeCu₂Si₂, isotypic with ThCr₂Si₂, has been refined in a single-crystal study. The atomic parameters were used in self-consistent LMTO band structure calculations for CeCu₂Si₂ and isostructural LaCu₂Si₂. The results are analysed in terms of energy levels, charge distribution and in particular Fermi surface properties. The Ce-4f levels are situated mainly aboveE _F , except near the Γ-point. The density-of-states atE _F is large and heavily concentrated around the Ce-4f band. This makes local Ce 4f fluctuations possible, while interaction with the rest of the band structure is small. The comparison with LaCu₂Si₂ shows that the additional Cef electron is partly promoted into the non-f bands. Large enhancement factors are required to bring band results into agreement with observed specific heat and magnetic critical field. Strong Fermi surface anisotropies are pointed out for both compounds suggesting new experiments on single crystals.     

Thermodynamic properties of CeCu6-xAux: Fermi-liquid vs. non-Fermi-liquid behaviour

We report on a detailed comparison of the thermodynamic properties of the heavy-fermion system CeCu₆ which can be described as a Fermi liquid at low temperatures T < 0.1 K, and CeCu_5.9Au_0.1 where strong deviations from the Fermi-liquid behaviour were found previously in the T dependence of the specific heat C, magnetization M and electrical resistivity p. The specific heat, magnetization and elastic constants are investigated in a large range of magnetic fields, corroborating the idea that the non-Fermi-liquid behaviour arises from low-lying spin excitations. For the elastic constants, a striking linear T dependence is found for CeCu_5.9Au_0.1 in contrast to the T² Fermi-liquid behaviour of CeCu₆.     

Crystal-field excitations in the heavy-fermion alloys CeCu6−x Au x studied by specific heat and inelastic neutron scattering

The specific heat of CeCu_6–x Au _x withx=0,0.3, and 0.9, and of the corresponding La homologues has been measured between 1.5 K and 150 K. With increasingx we find progressively better-defined Schottky anomalies arising from the crystal-field splitting, which is attributed to the decrease of the Kondo temperature. Both observations are in line with the results of inelastic neutron-scattering data performed on samples withx=0.5. Overall, the crystal-field splitting does not change very much upon alloying with Au. A detailed analysis shows that forx=0.5 the quasielastic line width is smaller and the inelastic crystal-field transitions are better resolved compared to CeCu₆.     

Fermi-liquid instability at magnetic–nonmagnetic quantum phase transitions

In metals with strong electronic correlations such as heavy-fermion systems or itinerant-electron magnets it is possible to change from a magnetically ordered to a nonmagnetic groundstate by variation of an external parameter such as composition or pressure. In principle a transition between these groundstates can occur at zero temperature. In case of a continuous transition quantum fluctuations take the role of thermal fluctuations in finite-temperature transitions. The abundance of low-lying magnetic excitations leads in the vicinity of the quantum critical point to unusual behavior of thermodynamic and transport properties at low temperatures T not envisioned by the classical Fermi-liquid behavior that is observed even in strongly correlated electron systems away from the quantum phase transition. We discuss in detail a few examples of this ‘non-Fermi-liquid behavior', viz., CeCu_6−xAu_x, Ce_1−xLa_xRu₂Si₂, Ce₇Ni₃, CeCu₂Si₂ and CeCu₂Ge₂, CePd₂Si₂, and UCu_1−xPd_x. In CeCu_6−xAu_x the very unusual low-T behavior of the linear specific-heat coefficient C/T−ln(T/T₀) and of the resistivity ΔρT can be attributed to quasi-two-dimensional fluctuations as determined from inelastic neutron scattering. The systems CeCu₂Ge₂ and CePd₂Si₂ are particuarly interesting since here the magnetic order which is suppressed under hydrostatic pressure gives way to superconductivity, suggesting that spin fluctuations mediate the formation of Cooper pairs at least in the latter system.     

Transport properties of LaCu2Si2 and CeCu2Si2 between 1.5K and 300K

We report measurements of the electrical resistivity, the thermal conductivityk and the thermoelectric powerS between 1.5K and 300K on the anomalous CeCu₂Si₂ compound and on LaCu₂Si₂ as reference compound. For LaCu₂Si₂ the temperature dependences of andS are in accord with those found in otherd band metals. For CeCu₂Si₂ the observed resistivity (220 µ cm at 200K) leads to a very short electronic mean free path which is of the order of the Ce-Ce spacing. Correspondingly,k is almost identical with the phonon contributionk _p . Below 20K, resistivity and thermoelectric power strongly suggest Fermi liquid behavior with a degeneracy temperature between 20K and 40K. Above 200K, both andS decrease proportionally to –ln(T/1 K).Work performed within the research program of the Sonderforschungsbereich 125 Aachen/Jülich/KölnPart of this work will be presented at the Int. Conf. on Rare Earths in the Metallic State, St. Pierre de Chartreuse, Sept. 1978     

Dynamics of the magnetization in the heavy fermion system CeCu6

We have studied CeCu₆ by inelastic neutron scattering. We found both quasielastic and also inelastic transitions, which we interpret as residual crystal field transitions. The quasielastic linewidth is a strongly nonlinear function of temperature, with approximately _QE=5.0 meV at 300 K, with a crossover _QE=kT at about 13 K and with a residual value of _QE=(0)=0.50 meV forT=0 K. Below 5 K the quasielastic intensityI _QE decreases linearly with temperature. _stI _QE/T is in good agreement with direct measurements of the static susceptibility. The data are fully consistent with a nonordering groundstate of CeCu₆.     

Structural and magnetic properties of RET2Sn2 compounds (RE=La,Ce, Sm; T=Ni,Cu)

The following compounds have been synthesized: LaCu₂Sn₂, CeCu₂Sn₂, SmCu₂Sn₂ and SmNi₂Sn₂. By means of X-ray diffraction their structure was determined to be primitive tetragonal of CaBe₂Ge₂-type (space group P4/nmm) and the lattice parameters were obtained.¹¹⁹Sn Mössbauer measurements were performed in a temperature range between 4.2 K and 300 K. The temperature dependence of the Lamb-Mössbauer factor reveals considerable softening of lattice vibration modes below 160 K. Only SmCu₂Sn₂ orders magnetically above 4.2 K.     

Structural and magnetic properties of Ce(Cu,Ni)2 pseudobinary phases

The stability of the pseudobinary phases obtained by partial substitution of Ni with Cu, Ag or Au in the cubic Laves phase CeNi₂, or by partial substitution of Cu with Ni in the orthorhombic compound CeCu₂ has been investigated. No solid solubility of Cu, Ag and Au in the CeNi₂ cubic lattice could be detected. In contrast, pseudobinary orthorhombic phases, corresponding to the formula CeCus_2?xNi_x, exist over the range x = 0 to 1. For these phases, crystal structures and magnetic properties have been determined. In every case, the electronic configuration of cerium appears to be unaffected to the Ni content, and corresponds to the trivalent state. The Ni atoms are in a non-magnetic state. The magnetic susceptibility of CeCu₂ in the region from 530 to 900 K shows anomalous behaviour, which should be due to a metamagnetic transition.     

Electron spin resonance investigation of the Heavy-Fermion compound CeCu2(Si1−x Ge x )2

The Kondo-lattice system CeCu₂(Si_1?x Ge _x )₂ exhibits an alloying induced transition from a coherent Fermi-liquid (x=0) with strongly enhanced effective masses to an antiferromagnetically ordered heavy-fermion system (x=1). This transition is studied by Gd³⁺ ESR in oriented powder samples. The temperature dependence of the ESR line width follows a characteristic pattern which allows one to distinguish between the different ground states. The results obtained in polycrystalline CeCu₂Si₂ are in good agreement with the measurements performed in single crystals. Finally we compare our results with⁶³Cu-NMR data obtained from CeCu₂Si₂ and CeCu₂Ge₂.     

First-principles studies of the structural,elastic, and lattice dynamical properties of ZrMo2 and HfMo2

A comprehensive investigation of the structural, elastic, and lattice dynamical properties for ZrMo₂ and HfMo₂ with C14, C15, C36, and CeCu₂ phases are conducted using density functional total energy calculations. The results have showed that C15 phase for both materials is energetically more stable than C14, C36 and CeCu₂ phases. We have also estimated the mechanical behaviours of these compounds, including mechanical stability, bulk modulus, Young's modulus, shear modulus, Poisson's ratio, ductility, and anisotropy. Additionally, the lattice dynamical properties are analyzed and discussed exhaustively for these phases. The calculated properties agree well with available experimental and theoretical data.     

Competing polarization mechanisms in the heavy-fermion paramagnet CeCu<Subscript><Emphasis Type="Bold">6</Emphasis></Subscript>

Nuclear magnetic resonance (NMR) and relaxation of ⁶³Cu and ⁶⁵Cu in a powder sample of the heavy-fermion paramagnet CeCu₆ is measured and analysed quantitatively. Five different Cu sites are accessible to a detailed analysis. We derive quadrupolar splitting frequencies, Ce to Cu transferred hyperfine field coupling constants, and transversal as well as longitudinal relaxation behaviour. Only small relaxation anomalies are observed at the orthorhombic to monoclinic structural phase transition of CeCu₆. We point to the different importance of transferred hyperfine interaction and local conduction electron density for static or dynamic part, respectively, of Cu hyperfine interaction. The different sign of the transferred hyperfine interaction from Ce³⁺ to different Cu neighbours reveals the different competing interaction mechanisms, giving rise to the heavy-fermion paramagnetic behavior of CeCu₆. Received 20 November 2001     

Coexistence model of anisotropic electron hole pairing and unconventional superconductivity in Heavy Fermion compounds

Various Heavy Fermion compounds exhibit unconventional superconductivity together with another electronic instability like a spin density wave or possibly a more general type of anisotropic electron-hole pairing, e.g. a spin nematic state. The coexistence behaviour of these order parameters is studied within a simple weak coupling model. It is found that depeding on the symmetry of the order parameters coexistence or phase expulsion may occur. Whereas the former case is possibly realized for theU-based superconductors, CeCu₂Si₂ may be an example of the second case as observed and discussed in the context of elastic constant anomalies.     

Synchrotron X-ray diffraction and absorption studies of CeM2X2 (M=Cu, Ni and X=Si, Ge) at high pressure

The equations of state of CeCu₂Si₂ and CeCu₂Ge₂ to about 60 GPa, as well as that of CeNi₂Ge₂ to 22 GPa and the valence state of Ce in CeCu₂Ge₂ to 20 GPa have been studied at room temperature in a diamond-anvil cell using synchrotron radiation sources. In each compound, the ambient-pressure phase (tetragonal ThCr₂Si₂-type structure) persisted to the highest pressure studied. The unit cell volumes of CeNi₂Ge₂ at ∼5 GPa and CeCu₂Ge₂ at ∼7 GPa, respectively, approached that of CeCu₂Si₂ taken at ambient pressure. From the equation-of-state data, the bulk modulus was derived to be 112.0±5.1 GPa for CeCu₂Si₂, 125.6±4.3 GPa for CeCu₂Ge₂, and 178.4±14.3 GPa for CeNi₂Ge₂. The valence state of Ce in CeCu₂Ge₂ remained trivalent throughout the pressure range investigated.     

Metals near a magnetic instability

Zero-temperature magnetic phase transitions exhibit an abundance of nearly critical magnetic fluctuations that allow to probe the traditional concepts of the metallic state. For the prototypical heavy-fermion compound, CeCu_6−x Au _x , a breakdown of the Fermi-liquid properties may be tuned by Au concentration, hydrostatic pressure, or magnetic field. The d-electron weak itinerant ferromagnet ZrZn₂, on the other hand, was recently found to display superconductivity in coexistence with ferromagnetism.     

重费密子系统CeCu6-xNix的极低温电阻研究

CeCu₆是一种重费密子系统,采用Ni替代Cu研究磁性原子掺杂的多晶样品CeCu_6-xNi_x(x=0.00,0.05,0.10,0.15,0.20)在极低温下的电阻随温度的变化规律.实验结果表明,随着Ni原子掺杂量的增加,电阻的规律发生变化.在500mK以下,x≈0.1的样品电阻与温度呈线性关系,表现出非费密液体行为,而其他样品皆为典型的费密液体,x≈0.1是其临界掺杂成分.对比用Au替代的情况,临界掺杂成分也是0.1,但Au掺杂是靠体积膨胀来改变合金的基态性质,而Ni掺杂则是因其磁性造成对合金基态性质的影响 关键词： 重费密子 临界掺杂 非费密液体     

Specific features of the electronic structure of the CeCu<Subscript>6</Subscript>, CePd<Subscript>3</Subscript>, CeSi<Subscript>2</Subscript>, and CeF<Subscript>3</Subscript> systems

The electronic structure of cerium systems, the hybridization of 4 f and outer-shell electrons, and the influence of the position of the localized 4 f level with respect to the Fermi level E _F in the conduction band have been investigated. The CeCu₆, CePd₃, CeSi₂, and CeF₃ systems have been studied using X-ray photoelectron spectroscopy. The densities of states have been calculated by the tight-binding linearized muffin-tin orbital method within the atomic sphere approximation, which takes into account the covalent character of bonds and the nonspherical distribution of the electron density. The results obtained from the calculations of the total density of states are in good agreement with the valence band X-ray photoelectron data for the systems under investigation. It has been shown that the differences in the properties of the cerium systems are determined by the specific features of their electronic structure. A strong interatomic interaction is characteristic of heavy-fermion systems.