Magnetism and superconductivity in intermetallic uranium compounds

Superconductivity, spin-fluctuation effects and magnetic order are reviewed for intermetallic compounds of uranium with d-transition elements. Large values for the effective mass of the pairing electrons are deduced from critical field studies on the superconducting compounds. Magnetism in the 5f-electron compounds is strongly anisotropic even for paramagnetic materials. Magnetic order does not frequently occur in these intermetallics, spin fluctuations are often observed. A unique combination of spin-fluctuation phenomena and superconductivity is met in UPt₃.     

Structure and superconductivity of La1.8Sr0.2CuO4 and multi-phase Y1.2Ba0.8CuO4 under high pressure

Superconducting La_1.8Sr_0.2CuO₄ has been investigated under pressure. Its resistiveT _c -midpoint was found to be 37 K at ambient pressure. It inductively determinedT _c is 33 K monotonically shifting up to 38.4 K at 19.2 kbar. The initial linear increase is 0.295 K/kbar. X-ray investigations in a diamond anvil revealed no phase transformation of the K₂NiF₄ structure up to about 50 kbar at 300 K, 60 K and 15 K. The bulk modulus of La_1.8Sr_0.2CuO₄ was 1070 kbar at 300 K and 1500 kbar at 15 K. Thec/a ratio decreases and shows pronounced differences between room temperature and low temperature data under pressure. Multi-phase Y–Ba–Cu-Oxide with resistiveT _c -onset of 90 K was investigated under pressure, too. The inductive transition starts at 70 K and is completed at 20 K. The superconducting volume fraction was estimated to be about 2% at 10 K.     

Effect of magnetic field on AF correlations in UPt<Subscript>3</Subscript>

Following our recent suggestion that antiferrmagnetism of UPt₃ can be understood within the crystal field splitting scheme and that the observed below 5 K AF correlations are dominated by thermal fluctuations, we examine here the effect of a uniform magnetic field on these correlations. Orientations of field in the basal plane and perpendicular to it are considered. The field of a few teslas must have a pronounced effect which can be used as a check of the suggested scheme.     

Dielectric observation of a probably antiferroelectric high pressure phase in the ferroelectric Tris-Sarcosine Calcium Chloride (TSCC)

Dielectric susceptibility and ferroelectric hysteresis measurements on TSCC show that the 2nd-order paraelectric-ferroelectric (PE-FE) phase boundary beginning at (130.8 K, 1 bar) runs with pronounced curvature to (176.8 K, 5.03 kbar), where a new phase of low dielectric susceptibility appears. This phase is hypothesized to be antiferroelectric (AFE) with 3 possible structures: orthorhombic (P2₁2₁2₁, piezoelectric) or monoclinic ($\text{P2}{}_1\text{a}$ or $\text{P2}{}_1\text{n}$, centrosymmetric). The FE-AFE phase boundary was determined down to (81.0 K, 2.60 kbar) and the PE-AFE boundary up to (225.5 K, 6.82 kbar). Both the FE-AFE and PE-AFE transitions are of 1st order over the range studied.     

Observation of the Meissner effect in the high-Tc (pressure-) phase of the organic superconductor β-(BEDT-TTF)2I3

It is shown that the recently found superconducting state below 6 K in β-(BEDT-TTF)₂I₃ under a pressure of 1.5 kbar is diamagnetic and exhibits Meissner effects of up to 24 %, indicating that superconductivity is a true volume effect in these crystals. In contrast, no traces of diamagnetism are found in iodine doped α-(BEDT-TTF)₂I₃, for which resistively observed superconducting transitions in the vicinity of 3 to 5 K have also been reported.     

Mössbauer studies of neptunium intermetallics at high pressure

Using the 60keV Mössbauer transition in²³⁷Np high pressure experiments have been performed up to 85kbar between 4.2K and 200K on NpCo₂Si₂, NpAl₂, NpOs₂ and NpAs. The delocalization of 5f-electrons with reduced volume is most pronounced in NpOs₂ and NpAl₂, whereas NpCo₂Si₂ can be considered as a highly localized magnet. In NpAs 5f-hybridization with electrons of As is dominant. At pressures above 25kbar a new magnetic phase is formed.This work has been funded by the German Federal Minister for Research and Technology (BMFT) under contract Nr. 03-KA1TUM-4.     

1H NMR study of [N(CH3)4]2ZnCI4 at high pressures and low temperatures

Wide-line proton NMR studies on polycrystalline tetramethylammonium tetrachlorozincate have been carried out at high hydrostatic pressures up to 15 kbar in the temperature range 77-300 K and at ambient pressure down to 4.2 K. A second-moment transition is observed to occur starting around 161 K, the temperature for the V-VI phase transition. This transition temperature is seen to have a negative pressure coefficient up to 2 kbar, beyond which it changes sign. At 77 K the second moment decreases to 4 kbar and then increases again as a function of pressure. The results are explained in terms of the dynamics of the N(CH₃)₄ groups.     

Effect of hydrostatic pressure on the Curie temperature of the Heusler alloys Ni2MnZ(Z = Al,Ga, In,Sn and Sb)

The pressure derivative of the Curie temperature dT_c/dp of the Heusler alloys Ni₂MnZ(Z = Al, Ga, In, Sn and Sb) has been obtained from the results of temperature dependence of initial permeability under pressure up to about 6 kbar. For all alloys the Curie temperatures increase linearly with increasing pressure at the rate of dT_c/d_p: +0.7 K/kbar for Ni₂MnAl, +1.0 K/kbar for Ni₂MnGa, +0.9 K/kbar for Ni₂MnIn, +1.4 K/kbar for Ni₂MnSn and +4.1 K/kbar for Ni₂MnSb. On the basis of these results, the interatomic dependence of the exchange interaction for Heusler alloys is discussed. The magnetic susceptibilities of those alloys are also reported.     

Compression and polymorphism of potassium to 400 kbar

Both the compression and polymorphism of K were investigated to about 400 kbar at room temperature in a diamond-anvil pressure cell by optical and X-ray diffraction techniques. The ambient b.c.c.-K(I) is stable to about 120 kbar. The compression data for K(I), fitted to the Birch equation of state, yielded the zero-pressure bulk modulus B₀ = 29.9 ± 0.2 kbar and its first pressure derivative B'₀ = 4.15 ± 0.10. These values agree very well with those of recent data derived from the direct measurement of length changes using piston-displacement (to 20 kbar) and laser interferometer (to 7 kbar) techniques. On the basis of the compression data for K(I) alone, Bridgman's pressure scale may be overestimated by about 10 kbar at 100 kbar and that of Kennedy and LaMori may be underestimated by about 5 kbar at 50 kbar. Two high-pressure polymorphs of K were revealed in the pressure range 100–200 kbar. The b.c.c. → f.c.c. transition in K was observed to occur near 120 kbar, accompanied by a −2.5% discontinuous change in volume. The sample changes gradually from silver to gold in the range 130–150 kbar. The f.c.c.-K.(II) transforms further into an as yet undetermined structure between 170 and 190 kbar. No change in colour was observed in the latter transition. K(III) is stable up to at least about 400 kbar. The equation of state for the f.c.c. phase of K cannot be established. The volume of K was compressed more than 60% in the vicinity of 200 kbar, however.     

Pressure induced resonance of the Raman linewidth of the A1 mode of Cu3V S4

Investigations of the Raman spectrum of Cu₃V S₄ under pressure up to 60 kbar show a pronounced enhancement of the linewidth of the A₁ mode around 20 kbar. This anomaly is interpreted in terms of a resonance between the A₁ mode and a double phonon structure arising from the combination of F₂ like zone center phonons.     

High pressure effect on the electrical properties of NiS2

A semiconductor-metal transition in the electrical resistance of NiS₂, which has been suggested to be a Mott transition, is observed with decreasing temperature under pressure up to 44 kbar. The transition temperature increases with pressure with a slope of $\text{dT}\text{dP}\text{= 6 ± 1 K/kbar}$. The activation energy in a semiconducting region is found to decrease with increasing pressure and to vanish at about 46 kbar. The critical pressure and temperature are predicted to be 46 ± 2 kbar and 350 ± 20 K.     

Pressure effect on the anomalous electrical conductivity of magnetite

The temperature dependence of the electrical conductivity of magnetite was measured under hydrostatic pressure up to 18.4 kbar. It is found that the temperature of the conductivity maximum in the high temperature phase is more rapidly reduced by pressure (dT_m/dP = -4.1 K/kbar) than the Verwey temperature (dT_v/dP = -0.27 K/kbar). The discontinuous change of the conductivity at T_v appears to increase with applied pressure as a result of a lowering of T_m.     

Pressure-induced magnetic transition in Fe2P

The weak field ac susceptibility and the resistivity of Fe₂P single crystals were measured as functions of temperature from 4.2–300 K and as functions of hydrostatic pressures up to 20 kbar, using a newly designed clamp-type pressure cell. The Curie temperature, and the first-order transition temperature, decreased rapidly with increasing pressure, and ferromagnetism vanished at about 13 kbar at 0 K. A second-order transition temperature, as well as the first-order transition, appeared in the region below 170 K and above 5 kbar (triple point) and a new pressure-induced magnetic phase was found. The phase is proposed to be antiferromagnetic for reasons discussed in the paper.     

Changes of valence state of Yb in YbCuAl at high pressure: A Mössbauer study

The 84.3 keV Mössbauer transition in¹⁷⁰Yb was used to investigate the intermediate valent intermetallic compound YbCuAl at pressures up to 130 kbar and in the temperature range between 1.6 K and 77 K. The electric quadrupole interaction parameters |eQV _zz | and , as well as their temperature variation are drastically dependent on pressure: |eQV _zz | is at 4.2 K larger by almost a factor of three at 130 kbar when compared to ambient pressure. On the other hand, |eQV _zz | drops by more than a factor of two at 130 kbar when the temperature is raised from 1.6 K to 77 K. A much smaller temperature dependence of quadrupole coupling is present at ambient pressure. Both these effects give strong evidence for a valence transition towards the 4f ¹³ (Yb³⁺) configuration under applied pressure. At 4.2 K this transition is completed near 50 kbar. No magnetic order could be detected down to 1.6 K over the whole pressure range. Some line broadening is observed at high pressures and low temperatures which most probably is related to paramagnetic relaxation phenomena and supports the claim that the Yb ion is in a magnetic state under these conditions.Work supported by the Deutsche Forschungsgemeinschaft     

Hybridization,electronic structure and properties of uranium intermetallics: URu3, URh3, UPd3, UIr3 and UPt3

Results of fully-relativistic local density energy band calculations for uranium intermetallics, URu₃ URh₃, UPd₃, UIr₃ and UPt₃, are presented. These include energy bands projected by angular momentum and atom type, total and projected densities of states, specific heat mass enhancement factors and Stoner factors, Systematic variations in hybridization between uranium and transition-metal (X) states,particularly U-f and X-d, are found. The effects of crystal structure on the electronic structure of UPt₃ are examined. The f-d hybridization in the observed hexagonal UPt₃ phase is larger than that in the cubic phase. It is shown by inspecting the wavefunctions on the Fermi surface that the large k-dependence of the hybridization results in strong anistropy of the Fermi surface.     

Hydrostatic pressure study of the structural phase transitions and superconductivity in single crystals of (Ba1−xKx)Fe2As2 (x=0 and 0.45) and CaFe2As2

We studied the effect of hydrostatic pressure (P) on the structural phase transitions and superconductivity in the ternary and pseudo-ternary iron arsenides CaFe₂As₂, BaFe₂As₂, and (Ba_0.55K_0.45)Fe₂As₂, by means of measurements of electrical resistivity (ρ) in the 1.8-300 K temperature (T) range, pressures up to 20 kbar, and magnetic fields up to 9 T. CaFe₂As₂ and BaFe₂As₂ (lightly doped with Sn) display structural phase transitions near 170 and 85 K, respectively, and do not exhibit superconductivity in ambient pressure, while K-doped (Ba_0.55K_0.45)Fe₂As₂ is superconducting for T<30 K. The effect of pressure on BaFe₂As₂ is to shift the onset of the crystallographic transformation down in temperature at the rate of ~−1.04 K/kbar, while shifting the whole ρ(T) curves downward, whereas its effect on superconducting (Ba_0.55K_0.45)Fe₂As₂ is to shift the onset of superconductivity to lower temperatures at the rate of ~−0.21 K/kbar. The effect of pressure on CaFe₂As₂ is first to suppress the crystallographic transformation and induce superconductivity with onset near 12 K very rapidly, i.e., for P<5 kbar. However, higher pressures bring about another phase transformation characterized by reduced-resistivity, and the suppression of superconductivity, confining superconductivity to a narrow pressure dome centered near 5 kbar. Upper critical field (H_c2) data in (Ba_0.55K_0.45)Fe₂As₂ and CaFe₂As₂ are discussed.     

Effect of pressure on the Kondo temperatures of Au(Fe) and Au(Mn)

The electrical resistivity of four Kondo systems, Au-(5 p.p.m. Fe), Au-(39 p.p.m. Fe), Au-(17 p.p.m. Mn) and Au-(50 p.p.m. Mn) has been measured in the temperature range 1.3–20 K at pressures up to 80 kbar. The Kondo temperature T_K is found to increase initially with pressure at the rate of 1.1%/kbar for Au(Fe) and 6%/kbar for Au(Mn). The volume dependence of the effective exchange constant J_eff is derived.     

Pressure induced superconductivity in BaMo6S8

The resistance and a.c. magnetic susceptibility of BaMo₆S₈ have been measured under pressure. A resistance-anomaly, indicative of the reported structural transformation at ～ 145 K, was observed. Non-bulk superconductivity with a pressure dependent signal size was induced by a quasi-hydrostatic pressure ? 15 kbar but not a hydrostatic pressure up to 18 kbar down to 1.2 K.     

Spinfluctuations versus phonons: The case of Heavy-Fermion superconductivity

Superconductivity of Heavy-Fermions, with an emphasis on hexagonal UPt₃, is investigated microscopically on the basis of the LNCA-approximation for strongly correlated electrons in a Kondo lattice and of Eliashberg theory for anisotropic singlet and triplet superconducting order. The effective interaction kernel incorporates exchange of spin fluctuations carried by strongly renormalized particle-hole excitations as well as exchange of phonons generated by the breathing mechanism. Particular care is taken to include realistic anisotropies in band structure and couplings and to expand interaction kernel and order parameter in appropriate Fermi surface harmonics. Separate interactions and corresponding gap equations are used for pseudo-spin-singlet and -triplet channel, with a restriction to the case of weak spin-orbit coupling. Our main results include a detailed study of phonon- and spin-fluctuation mechanisms as a possible source for superconductivity and, in combination, their mutual influence and competition. Furthermore, the questions regarding singlet or triplet order, conventional or unconventional symmetry, order parameter zeros and phase transitions between different superconducting states are addressed. We propose a possible scenario of Heavy-Fermion superconductivity.     

High pressure study on TiBe2−x Cux and ZrZn2

The Curie temperature of the itinerant ferromagnets TiBe_2?xCu_x was found to decrease linearly with pressure up to 20 kbar. No sign of superconductivity was detected in TiBe_2?x Cu_x and ZrZn_1.9 up to 90 kbar and down to 1.2K. The results are discussed in terms of the model recently suggested by Enz and Matthias concerning the occurence of magnetism and p-state superconductivity in these compounds.