Extended stability range of the non-Fermi liquid phase in UCoAl.

High pressure was used to investigate the stability of the non-Fermi liquid (NFL) state, observed in electrical resistivity of uranium-based band metamagnet UCoAl in a pure form (paramagnet) or with Fe substitution (ferromagnetic ground state), both in a single-crystal form. By combining the pressure variations of magnetization and resitivity in these materials the phase diagram for UCoAl had been constructed. The band metamagnet transforms into the ferromagnetic state as the critical metamagnetic field is reduced to zero by the lattice expansion analogous to the negative pressure. Within the same diagram, the increasing hydrostatic pressure drives the critical metamagnetic field upwards while reducing the magnetization increment at the transition. The NFL state persists to about 4-5 GPa. Although spin fluctuations play an important role in the character of UCoAl, they do not exhibit any criticality in the sense of divergence of parameters describing the resistivity around the Ferro-NFL phase transition, which is of the first order type.

Electronic properties of Pu19Os simulating ß-Pu: the strongly correlated Pu phase.

We established the basic electronic properties of ζ-Pu19Os, which is a close analogue to ß-Pu, and its low-temperature variety, η-Pu19Os. Their magnetic susceptibility is 15% higher than for δ-Pu. A specific heat study of ζ-Pu19Os shows a soft lattice similar to δ-Pu, leading to a low Debye temperature Θ D = 101 K. The linear electronic coefficient γ related to the quasiparticle density of states at the Fermi level points to a higher value, 55 ± 2 mJ (mol Pu K2)-1, compared to 40 mJ (mol K2)-1 for δ-Pu. The results confirm that ß-Pu is probably the most strongly correlated Pu phase, as had been indicated by resistivity measurements. The volume and related Pu-Pu spacing is clearly not the primary tuning parameter for Pu metal, as the ß-Pu density stands close to the ground-state α-phase and is much higher than that for δ-Pu. The η-Pu19Os phase has a record γ-value of 74 ± 2 mJ (mol Pu K2)-1. The enhancement is not reproduced by LDA+DMFT calculations in the fcc structure, which suggests that multiple diverse sites can be the key to the understanding of ß-Pu.

Probing Magnetism in the Vortex Phase of PuCoGa_{5} by X-Ray Magnetic Circular Dichroism.

We measure x-ray magnetic circular dichroism (XMCD) spectra at the Pu M_{4,5} absorption edges from a newly prepared high-quality single crystal of the heavy-fermion superconductor ^{242}PuCoGa_{5}, exhibiting a critical temperature T_{c}=18.7 K. The experiment probes the vortex phase below T_{c} and shows that an external magnetic field induces a Pu 5f magnetic moment at 2 K equal to the temperature-independent moment measured in the normal phase up to 300 K by a superconducting quantum interference device. This observation is in agreement with theoretical models claiming that the Pu atoms in PuCoGa_{5} have a nonmagnetic singlet ground state resulting from the hybridization of the conduction electrons with the intermediate-valence 5f electronic shell. Unexpectedly, XMCD spectra show that the orbital component of the 5f magnetic moment increases significantly between 30 and 2 K; the antiparallel spin component increases as well, leaving the total moment practically constant. We suggest that this indicates a low-temperature breakdown of the complete Kondo-like screening of the local 5f moment.

Tricritical point from high-field magnetoelastic and metamagnetic effects in UN.

Uranium nitride (UN) is one of the most studied actinide materials as it is a promising fuel for the next generation of nuclear reactors. Despite large experimental and theoretical efforts, some of the fundamental questions such as degree of 5 f-electron localization/delocalization and its relationship to magneto-vibrational properties are not resolved yet. Here we show that the magnetostriction of UN measured in pulsed magnetic fields up to 65 T and below the Néel temperature is large and exhibits complex behavior with two transitions. While the high field anomaly is a field-induced metamagnetic-like transition and affects both magnetisation and magnetostriction, the low field anomaly does not contribute to the magnetic susceptibility. Our data suggest a change in the nature of the metamagnetic transition from first to second order-like at a tricritical point at T tri ∼ 24 K and H tri ∼ 52 T. The induced magnetic moment at 60 T might suggest that only one subset of magnetic moments has aligned along the field direction. Using the results obtained here we have constructed a magnetic phase diagram of UN. These studies demonstrate that dilatometry in high fields is an effective method to investigate the magneto-structural coupling in actinide materials.

Absence of superconductivity in fluorine-doped neptunium pnictide NpFeAsO.

X-ray diffraction, specific heat, magnetic susceptibility and inelastic x-ray scattering measurements on the transurarium oxypnictides NpFeAsO and NpFeAsO0.85F0.15 are presented. No superconductivity down to 2 K was observed upon fluorine doping, contrary to the structurally analogous rare-earth pnictides. No modification of the phonon density of states was observed upon doping with fluorine. We discuss our results in light of the latest experimental and theoretical studies on the role of phonons in the superconducting pnictide compounds.

Magnetic polarization of the americium J=0 ground state in AmFe(2).

Trivalent americium has a nonmagnetic (J=0) ground state arising from the cancellation of the orbital and spin moments. However, magnetism can be induced by a large molecular field if Am^{3+} is embedded in a ferromagnetic matrix. Using the technique of x-ray magnetic circular dichroism, we show that this is the case in AmFe_{2}. Since ⟨J_{z}⟩=0, the spin component is exactly twice as large as the orbital one, the total Am moment is opposite to that of Fe, and the magnetic dipole operator ⟨T_{z}⟩ can be determined directly; we discuss the progression of the latter across the actinide series.

A plutonium-based single-molecule magnet.

The magnetic properties of the 5f(5) [tris-(tri-1-pyrazolylborato)-plutonium(III)] complex have been investigated by ac susceptibility measurements, showing it to be the first plutonium single-molecule magnet; its magnetic relaxation slows down with decreasing temperature through a thermally activated mechanism followed by a quantum tunnelling regime below 5 K.

(237)Np Mössbauer effect study on NpFeAsO.

We report (237)Np Mössbauer measurements on NpFeAsO. The Np atoms were found to occupy only one crystallographic site. The value of the isomer shift (δ âˆ¼ 9.1 mm s(-1) versus NpAl2) indicates a 5f(4) electronic configuration (Np(3+) ions). The magnetic ordering of the Np sublattice below 60 K is established and the saturated ordered magnetic moment is determined to be 1.73µB at 3.6 K. The unique set of hyperfine parameters exclude a modulated magnetic structure or spin waves on the Np site. The neptunium magnetic moments µNp are found to lie along the tetragonal c-axis.

Strong-coupling d-wave superconductivity in PuCoGa5 probed by point-contact spectroscopy.

Superconductivity is due to an attractive interaction between electrons that, below a critical temperature, drives them to form Cooper pairs and to condense into a ground state separated by an energy gap from the unpaired states. In the simplest cases, the pairing is mediated by lattice vibrations and the wavefunction of the pairs is isotropic. Less conventional pairing mechanisms can favour more exotic symmetries of the Cooper pairs. Here, we report on point-contact spectroscopy measurements in PuCoGa(5), a moderate heavy-fermion superconductor with a record high critical temperature T(c)=18.5 K. The results prove that the wavefunction of the paired electrons has a d-wave symmetry, with four lobes and nodes, and show that the pairing is likely to be mediated by spin fluctuations. Electronic structure calculations, which take into account the full structure of the f-orbital multiplets of Pu, provide a hint of the possible origin of these fluctuations.

Localized 5f electrons in superconducting PuCoIn5: consequences for superconductivity in PuCoGa5.

The physical properties of the first In analog of the PuMGa(5) (M = Co, Rh) family of superconductors, PuCoIn(5), are reported. With its unit cell volume being 28% larger than that of PuCoGa(5), the characteristic spin-fluctuation energy scale of PuCoIn(5) is three to four times smaller than that of PuCoGa(5), which suggests that the Pu 5f electrons are in a more localized state relative to PuCoGa(5). This raises the possibility that the high superconducting transition temperature T(c) = 18.5 K of PuCoGa(5) stems from the proximity to a valence instability, while the superconductivity at T(c) = 2.5 K of PuCoIn(5) is mediated by antiferromagnetic spin fluctuations associated with a quantum critical point.

Low temperature heat capacity and magnetic properties of UF3.

The low temperature heat capacity of UF(3) has been measured using an adiabatic low temperature calorimeter in the temperature range from 10 to 350 K. These data are complemented at the lowest temperature region with data obtained with a Quantum Design PPMS-14 device in the temperature range from 0.5 to 20 K. Good agreement between both techniques has been found, and from these experimental results the absolute entropy of UF(3) at 298.15 K has been determined as 126.8 ± 2.5 J K(-1) mol(-1). On the basis of the specific heat data and the magnetization measurements performed on a SQUID device, a transition at 1.59 K attributed to Curie temperature of a ferromagnetic transition has been found in this study. This observation makes UF(3) a unique compound with an unusually low ferromagnetic ordering temperature.

Magnetic and electronic properties of NpFeGa5.

NpFeGa(5) single crystals prepared by the Ga-flux method have been investigated by magnetisation, specific heat and (237)Np Mössbauer spectroscopy measurements. An antiferromagnetic (AF) transition has been observed at T(N) ~114 K. The second AF transition which takes place at T* ~74 K has only been detected in the magnetisation data. A saturated ordered Np moment of 1.00(5) µ(B) and the occurrence of an Np(3 + ) charge state were inferred from the Mössbauer data. The angle between the Np ordered moment and the basal plane was shown to be ~17°, in good agreement with the value observed by neutron diffraction in the low temperature AF phase. The absence of change of the quadrupole interaction parameters at T* did not allow us to gain information on the Np moment reorientation at T*. The trend of the isomer shift along the NpTGa(5) series and the discrepancy between the Np moments determined by neutron diffraction and Mössbauer spectroscopy indicated a partial spatial delocalisation of the 5f electrons in NpFeGa(5).

Superexchange coupling and slow magnetic relaxation in a transuranium polymetallic complex.

{Np(VI)O2Cl2}{Np(V)O2Cl(thf)3}2 is the first studied example of a polymetallic transuranic complex displaying both slow relaxation of the magnetization and effective superexchange interactions between 5f centers. The coupling constant for Np(V)-Np(VI) pairs is 10.8 K, more than 1 order of magnitude larger than the common values found for rare-earth ions in similar environments. The dynamic magnetic behavior displays slow relaxation of magnetization of molecular origin with an energy barrier of 140 K, which is nearly twice the size of the highest barrier found in polymetallic clusters of the d block. Our observations also suggest that future actinide-based molecular magnets will have very different behavior to lanthanide-based clusters.

High pressure study of Pu(0.92)Am(0.08) binary alloy.

The phase transitions (by means of x-ray diffraction) and electrical resistivity of a Pu(0.92)Am(0.08) binary alloy were determined under pressure (up to 2 GPa). The evolution of atomic volume with pressure gives detailed information concerning the degree of localization of 5f electronic states and their delocalization process. A quasi-linear V = f(P) dependence reflects subtle modifications of the electronic structure when P increases. The electrical resistivity measurements reveal the very high stability of the δ phase for pressures less than 0.7 GPa, since no martensitic-like transformation occurs at low temperature. Remarkable electronic behaviours have also been observed. Finally, resistivity curves have shown the temperature dependence of the phase transformations together with unexpected kinetic effects.

Superconductivity in the americium metal as a function of pressure: probing the Mott transition.

High-pressure measurements of the resistivity of americium metal are reported to 27 GPa and down to temperatures of 0.4 K. The unusual dependence of the superconducting temperature (T(c)) on pressure is deduced. The critical field [H(c)(0) extrapolated to T=0] increases dramatically from 0.05 to approximately 1 T as the pressure is increased, suggesting that the type of superconductivity is changing as pressure increases. At pressures of approximately 16 GPa the 5f electrons of Am are changing from localized to itinerant, and the crystal structure also transforms to a complex one. The role of a Mott-type transition in the development of the peak in T(c) above 16 GPa is postulated.

Structural tuning of unconventional superconductivity in PuMGa5 (M=Co,Rh).

The superconducting properties of the recently discovered PuMGa5 (M=Co,Rh) superconductors, including the power law behavior of the specific heat, the evolution of the superconducting transition T(c) temperature with pressure, and the linear relation between T(c) and ratio of tetragonal lattice parameters c/a, are compared to those of the heavy fermion CeMIn5 (M=Co,Rh,Ir) unconventional superconductors. The striking similarity of the properties between the two families of superconductors suggests a common physics and a common (magnetically mediated) mechanism of superconductivity.