Electronic structure and magnetism of RPdIn compounds (R=La, Ce, Pr, Nd)

RPdIn (R = La-Nd) compounds were studied by means of magnetic susceptibility, specific heat and photoelectron spectroscopy measurements. The results prove that CePdIn is an antiferromagnetic Kondo lattice with T_N below 1.7 K. The Pr-based indide remains paramagnetic down to 1.7 K, and the lack of any magnetic ordering may be due to the presence of a singlet as the crystalline electric field ground state or/and strong hybridization between Pr 4f states and Pd 4d states. In turn, NdPdIn exhibits ferromagnetism below about 26 K. In contrast to CePdIn, for the Pr- and Nd-based compounds any significant enhancement of the electronic specific heat coefficient was observed.     

59Co NMR study of NdCo2, GdCo2, TbCo2 and HoCo2

We have observed the ⁵⁹Co spectra of the Laves phase Co compounds with Nd, Gd, Tb and Ho. We observe a spectrum consisting of a pair of lines for Nd, Tb and Ho compounds, because the Co sites are magnetically inequivalent in the presence of dipolar or pseudodipolar fields. For the heavy rare earth compounds, the magnitude of this splitting is comparable to the dipolar splitting produced by the neighboring spins, but for Nd it is much larger. The Nd compound is also anomalous in that the average hyperfine field is only 37.2 kOe while for the 3 heavy rare earth compounds it is about 60 kOe. The magnitude of the hyperfine field is discussed in terms of a simple model relating it to the cobalt moment and the rare earth spin.     

On the low-temperature thermal properties and low-energy Fermi excitations in CeNiSn

The thermal expansion of a single crystal of the intermetallic compound CeNiSn has been measured at low temperatures 0.3 K<T<12 K and in a magnetic field up to 8 T. A large anisotropy of the linear expansion is observed which is strongly influenced by the magnetic field. These data are interpreted within the theory explaining the origin of the quasigap in the heavy fermion spectrum of CeNiSn by the interplay between the heavy fermions and low-energy excitations in non-cubic Kondo lattices.     

Anisotropic magnetic exchange in orthorhombic RCu2 compounds (R = rare earth)

The magnetic excitations in the field induced ferromagnetic phase F3 of a NdCu₂ single crystal were investigated by means of inelastic neutron scattering experiments. A mean field model using the random phase approximation in connection with anisotropic magnetic bilinear R-R (R denotes a rare earth) exchange interactions is proposed to account for the observed dispersion. The relevance of this model to the analysis of the magnetic ordering process in other RCu₂ compounds is discussed. Received 21 April 1999     

Superposition-model analysis of rare-earth doped BaY 2 F 8

The energy level schemes of four rare-earth dopants (Ce 3+ , Nd 3+ , Dy 3+ , and Er 3+ ) in BaY 2 F 8 , as determined by optical absorption spectra, were fitted with a single-ion Hamiltonian and analysed within Newman's Superposition Model for the crystal field. A unified picture for the four dopants was obtained, by assuming a distortion of the F m ligand cage around the RE site; within the framework of the Superposition Model, this distortion is found to have a marked anisotropic behaviour for heavy rare earths, while it turns into an isotropic expansion of the nearest-neighbours polyhedron for light rare earths. It is also inferred that the substituting ion may occupy an off-center position with respect to the original Y 3+ site in the crystal.     

μSR investigations of UX3 compounds

We report on measurements of UX₃ compounds. The crystal structure of these compounds is of the cubic AuCu₃ type. Compounds with this structure show all relevant metallic behaviours. In our case we compared two groups of mixed crystals. Both of them move from local‐moment magnetism to paramagnetic behaviour but one group develops a heavy fermion state in between. This revised version was published online in July 2006 with corrections to the Cover Date.     

Magnetic properties of the hexagonal NdNi5 and NdCu5 compounds

Magnetization and resistivity measurements performed on the hexagonal NdNi₅ and NdCu₅ compounds are presented. For NdNi₅, magnetization was measured on a single crystal along the three main axes of the orthohexagonal cell. This compound orders ferromagnetically at T_c = 7 K, a being the easy magnetization axis. Quantitative analysis of the experimental data led to the determination of the 4f-Nd and 3d-Ni contributions to the magnetization. In particular crystal field parameters were determined which account for inelastic neutron scattering data. Two original features of the compounds magnetic behaviour due to crystal field effects are noted: i) in the basal plane a large anisotropy of the magnetic moment which strongly increases with the magnetic field between 11 and 130 kOe; ii) a large decrease of the Nd moment during the rotation toward the c axis driven by the field. NdCu₅ orders also ferromagnetically at 15 K. The Nd moment lies perpendicular to c, and its reduction by the crystal field seems smaller than in NdNi₅.     

Heavy fermions in high magnetic fields

A qualitative picture of the metamagnetic transition in the Anderson lattice model of heavy fermion Ce compounds is described and a strong coupling spin fluctuation theory of the high field state is presented. The field dependence of the minority spin quasiparticle mass is calculated and the onset of the metamagnetic transition with decreasing field is discussed. The theory of the high field state is extended to include Landau levels and the oscillatory behaviour of the spin self-energy as a function of the inverse applied field is investigated. For the heavy fermion model considered such oscillations of the self-energy lead to significant modifications in the standard theory of the de Haas - van Alphen effect. The possible relevance to anomalous experimental results on CeRu₂Si₂ is discussed.     

Spin and temperature dependence of the magnetic hyperfine field of Cd in the rare earth-aluminum Lavesphase compounds RAl2

Perturbed angular correlation spectroscopy has been used to investigate the combined magnetic and electric hyperfine interaction of the probe nucleus ¹¹¹Cd in ferromagnetically ordered rare earth (R)-dialuminides RAl₂ as a function of temperature for the rare earth constituents R=Pr, Nd, Sm, Eu, Tb, Dy, Ho and Er. In compounds with two magnetically non-equivalent Al sites (R=Sm, Tb, Ho, Er), the magnetic hyperfine field was found to be strongly anisotropic. This anisotropy is much greater than the anisotropic dipolar fields, suggesting a contribution of the anisotropic 4f-electron density to magnetic hyperfine field at the closed-shell probe nucleus. The spin dependence of the magnetic hyperfine field reflects a decrease of the effective exchange parameter of the indirect coupling with increasing R atomic number. For the compounds with the R constituents R=Pr, Nd, Tb, Dy and Ho the parameters B₄, B₆ of the interaction of the crystal field interaction have been determined from the temperature dependence of the magnetic hyperfine field. The ¹¹¹Cd PAC spectrum of EuAl₂ at 9 K confirms the antiferromagnetic structure of this compound.     

Magnetic relaxation in UCu4 + xAl8 - x

A quasielastic neutron scattering study has been performed on UCu_4+xAl_8-x, a system which reveals an alloying-induced transition from magnetic order to heavy-fermion behavior. The magnetic response can be described by a broad quasielastic Lorentzian for all concentrations. No crystal field excitations could be detected. Remarkably, the linewidth decreases with increasing hybridization strength and seems to be no measure of the Kondo lattice temperature T*. In addition, electron spin resonance (ESR) experiments were performed which revealed that, even in the heavy-fermion regime, spin fluctuations play an important role. Both experimental findings are in distinct contrast to cerium-based heavy fermion systems.     

Magnetic properties of strongly frustrated and correlated systems

While consequences of frustration of magnetic interactions are much studied in localized spin systems, much less studies have been performed on frustrated metallic systems. However, several effects of strong geometrical frustration in metallic correlated system have also been experimentally observed in rare-earth or transition metal compounds: coexistence of magnetic and non-magnetic sites in ordered magnetic structure, heavy fermion behaviour and anomalous Hall effect due to spin chirality are consequences of frustration. An overview of the experimental observations and of the proposed models is given. Other interesting effects due to magnetic frustration in metallic systems, which have been predicted theoretically, are also reviewed.     

Magnetic interactions and crystal field in RMg3 compounds (R = Ce,Pr, Nd)

We have carried out a study of magnetic properties, electrical resistivity and of crystal field excitations using inelastic neutron scattering, in cubic RMg₃ compounds with light rare earths R = Ce, Pr and Nd. The ground states are the Γ₇ and Γ₆ doublets for CeMg₃ and NdMg₃, which order at 3.5 and 6.5 K, respectively. PrMg₃ has the non-magnetic Γ₃ ground state and remains a Van Vleck paramagnet. The magnetic contribution to the resistivity has been separated. It allows us to evaluate the couplings between the 4f shell and the conduction band which is much larger for CeMg₃ than for the other compounds. The coupling constant Γ is negative in this case, as shown by an incipient Kondo effect in this compound.     

A crystal field investigation of the properties of RCuAs2 (R=Pr, Nd, Sm, Tb, Dy, Ho, Er and Yb)

A crystal field (CF) investigation of the magnetic properties and heat capacities of RCuAs₂ (R=Pr, Nd, Sm, Tb, Dy, Ho, Er and Yb) has been carried out using the observed average magnetic susceptibilities (1.8-300 K) of the title compounds. The CF parameters proposed for the systems show a systematic variation throughout the rare-earth series. Other physical properties dependent on the CF are also computed and compared with available experimental data. The experimental heat capacity data reported for a limited range of temperature agree well with computed heat capacity for all the compounds (except SmCuAs₂ and YbCuAs₂). CF J mixing was found to be appreciable for all the samples except YbCuAs₂.     

XMCD at LII,III edges of rare-earths: electric quadrupolar and dipolar effects

X-ray Magnetic Circular Dichroism (XMCD) at L_II,III edges of rare earths in rare earth–3d transition metal compounds is still a subject of study. We present experimental evidence of electric quadrupolar transitions at L_III and L_II edges of Er in the ErFe₂ Laves phase. These experimental results are compared with atomic calculation taking into account crystal electric field effects on the Er site. Received: 30 May 2001 / Accepted: 4 July 2001 / Published online: 5 October 2001     

First-principles study on the crystal, electronic structure and mechanical properties of hexagonal Al3RE (RE = La, Ce, Pr, Nd, Sm, Gd) intermetallic compounds

The structural properties, elastic properties and electronic structures of hexagonal Al₃RE intermetallic compounds are calculated by using first-principles calculations based on density functional theory. Since there exists strong on-site Coulomb repulsion between the highly localized 4f electrons of RE atoms, we present a combination of the GGA and the LSDA+U approaches in order to obtain the appropriate results. The GGA calculated lattice constants for the hexagonal Al₃RE intermetallic compounds are in good agreement with available experimental values. The results of cohesive energy indicate that these compounds can be stable under absolute zero Kelvin and the stability of Al₃Gd is the strongest in all of the hexagonal Al₃RE compounds. The densities of states for GGA and LSDA+U approaches are also obtained for the Al₃RE intermetallic compounds. The mechanical properties are calculated from the GGA method in this paper. According to the computed single crystal elastic constants, Al₃La, Al₃Sm and Al₃Gd are mechanically unstable, while Al₃Ce, Al₃Pr and Al₃Nd are stable. The polycrystalline elastic modulus and Poisson’s ratio have been deduced by using Voigt-Reuss-Hill (VRH) approximations, and the calculated ratio of bulk modulus to shear modulus indicates that Al₃La compound is ductile material, but Al₃Ce, Al₃Pr, Al₃Nd, Al₃Sm and Al₃Gd are brittle materials.     

Tetragonal distortion from cubic symmetry at lower temperatures in the Cs2NaLnCl6 compounds (elpasolites) with light lanthanides

Single crystal magnetization- and NMR-measurements show that the Cs₂NaLnCl₆ compounds with the light rare earth Ce and Nd, contrary to that with the heavy rare earth Ho, are tetragonally distorted from cubic symmetry at lower temperatures. Because of this distortion, detailed single crystal magnetization data are required in order to evaluate the Ln crystal-field level scheme. The size of the distortion is such that it splits the ground quadruplet of Nd⁺³ into doublets nearly two Kelvin apart.     

Spin fluctuations and magnetic order in the heavy fermion compound CePt2Sn2

We present zero and longitudinal field μ SR measurements of single crystal and polycrystalline specimens of the heavy fermion compound CePt₂Sn₂. Above 1 K the behaviour of the two samples is indistinguishable; the muon 1/T_1 increases with decreasing temperature until 25 K when it plateaus. The 1/T_1 relaxation rate differs strongly for the two cases below \sim\,0.8\ K. At 0.1 K a rate of about 20 μ s^-1 is seen in the polycrystal while in the single crystal it is only about 5 μ s^-1. Even more revealing is the fact that longitudinal field decoupling spectra at very low temperatures demonstrate an essentially static spin system to be present in the polycrystalline material while the single crystal shows definite dynamic spin properties. We conclude that, in the presence of the distortion, long range magnetic order occurs below 0.9 K while in tetragonal symmetry long range order is suppressed (probably due to frustration) and spin fluctuations remain for T\rightarrow0. This revised version was published online in July 2006 with corrections to the Cover Date.     

Crystal field spectroscopy by inelastic neutron scattering

We present a review of inelastic neutron scattering results on very diluted rare earth (RE)-Laves phases. A systematic investigation to study crystal electric fields, experienced by single rare earth ions in a metallic environment, was done on (RE,R)Al₂, with RE=Pr, Nd, Tb, Dy, Ho, Er, Tm andR=Sc, Y, La. We show the influence of the 4f-ions on the crystal fields as well as the influence of the host lattices. The rare earth atoms in ScAl₂ have been studied for the first time and most of the other alloys, with LaAl₂ and YAl₂ as hosts, have been studied for the first time with magnetic atom concentrations below 1 at% and/or with good resolution for low energy excitations. Furthermore we studied the dynamics of 4f-moments, which are coupled to the conduction electrons by determining the coupling constants. We present a comprehensive set of crystal field parameters and coupling constants from these systematic studies and discuss them qualitatively within the available theoretical models. The influence of magnetic atom concentration on crystal field spectra will be shown in part II.     

Structures and physical properties of R_2TX_3 compounds

Rare-earth compounds have been an attractive subject based on the unique electronic structures of the rare-earth elements. Novel ternary intermetallic compounds R2TX3 (R = rare-earth element or U, T = transition-metal element, X = Si, Ge, Ga, In) are a significant branch of this research field due to their complex and intriguing physical properties, such as magnetic order at low temperature, spin-glass behavior, Kondo effect, heavy fermion behavior, and so on. The unique physical properties of R2TX3 compounds are related to distinctive electronic structures, crystal structures, micro-interaction, and external environment. Most R2TX3 compounds crystallize in AlB2-type or derived AlB2-type structures and exhibit many similar properties. This paper gives a concise review of the structures and physical properties of these compounds. Spin glass, magnetic susceptibility, resistivity, and specific heat of R2TX3 compounds are discussed.