Avoided valence transition in a plutonium superconductor.

The d and f electrons in correlated metals are often neither fully localized around their host nuclei nor fully itinerant. This localized/itinerant duality underlies the correlated electronic states of the high-Tc cuprate superconductors and the heavy-fermion intermetallics and is nowhere more apparent than in the 5f valence electrons of plutonium. Here, we report the full set of symmetry-resolved elastic moduli of PuCoGa5--the highest Tc superconductor of the heavy fermions (Tc = 18.5 K)--and find that the bulk modulus softens anomalously over a wide range in temperature above Tc. The elastic symmetry channel in which this softening occurs is characteristic of a valence instability--therefore, we identify the elastic softening with fluctuations of the plutonium 5f mixed-valence state. These valence fluctuations disappear when the superconducting gap opens at Tc, suggesting that electrons near the Fermi surface play an essential role in the mixed-valence physics of this system and that PuCoGa5 avoids a valence transition by entering the superconducting state. The lack of magnetism in PuCoGa5 has made it difficult to reconcile with most other heavy-fermion superconductors, where superconductivity is generally believed to be mediated by magnetic fluctuations. Our observations suggest that valence fluctuations play a critical role in the unusually high Tc of PuCoGa5.

Multiconfigurational nature of 5f orbitals in uranium and plutonium intermetallics.

Uranium and plutonium's 5f electrons are tenuously poised between strongly bonding with ligand spd-states and residing close to the nucleus. The unusual properties of these elements and their compounds (e.g., the six different allotropes of elemental plutonium) are widely believed to depend on the related attributes of f-orbital occupancy and delocalization for which a quantitative measure is lacking. By employing resonant X-ray emission spectroscopy (RXES) and X-ray absorption near-edge structure (XANES) spectroscopy and making comparisons to specific heat measurements, we demonstrate the presence of multiconfigurational f-orbital states in the actinide elements U and Pu and in a wide range of uranium and plutonium intermetallic compounds. These results provide a robust experimental basis for a new framework toward understanding the strongly-correlated behavior of actinide materials.

Emergent antiferromagnetism out of the "hidden-order" state in URu2Si2: high magnetic field nuclear magnetic resonance to 40 T.

Very high field (29)Si-NMR measurements using a fully (29)Si-enriched URu(2)Si(2) single crystal were carried out in order to microscopically investigate the "hidden order" (HO) state and adjacent magnetic phases in the high field limit. At the lowest measured temperature of 0.4 K, a clear anomaly reflecting a Fermi surface instability near 22 T inside the HO state is detected by the (29)Si shift, (29)K(c). Moreover, a strong enhancement of (29)K(c) develops near a critical field H(c) ≃ 35.6 T, and the ^{29}Si-NMR signal disappears suddenly at H(c), indicating the total suppression of the HO state. Nevertheless, a weak and shifted (29)Si-NMR signal reappears for fields higher than H(c) at 4.2 K, providing evidence for a magnetic structure within the magnetic phase caused by the Ising-type anisotropy of the uranium ordered moments.

Superconducting pairs with extreme uniaxial anisotropy in URu2Si2.

We report magnetic field orientation-dependent measurements of the superconducting upper critical field in high quality single crystals of URu(2)Si(2) and find the effective g factor estimated from the Pauli limit to agree remarkably well with that found in quantum oscillation experiments, both quantitatively and in the extreme anisotropy (≈10(3)) of the spin susceptibility. Rather than a strictly itinerant or purely local f-electron picture being applicable, the latter suggests the quasiparticles subject to pairing in URu(2)Si(2) to be "composite heavy fermions" formed from bound states between conduction electrons and local moments with a protected Ising behavior. Non-Kramers doublet local magnetic degrees of freedom suggested by the extreme anisotropy favor a local pairing mechanism.

Observation of the hybridization gap and Fano resonance in the Kondo lattice URu2Si2.

The nature of the second-order phase transition that occurs in URu2Si2 at 17.5 K remains puzzling despite intensive research. A key question emerging in the field is whether a hybridization gap between the renormalized bands can be identified as the "hidden" order parameter. We report on the measurement of a hybridization gap in URu2Si2 employing a spectroscopic technique based on quasiparticle scattering. The differential conductance exhibits an asymmetric double-peak structure, a clear signature for a Fano resonance in a Kondo lattice. The hybridization gap opens well above 17.5 K, indicating that it is not the hidden order parameter. Our results put stringent constraints on the origin of the hidden order transition in URu2Si2 and demonstrate that quasiparticle scattering spectroscopy can probe the band renormalizations in a Kondo lattice via detection of a novel type of Fano resonance.

Electronic tuning and uniform superconductivity in CeCoIn5.

We report a globally reversible effect of electronic tuning on the magnetic phase diagram in CeCoIn(5) driven by electron (Pt and Sn) and hole (Cd, Hg) doping. Consequently, we are able to extract the superconducting pair breaking component for hole and electron dopants with pressure and codoping studies, respectively. We find that these nominally nonmagnetic dopants have a remarkably weak pair breaking effect for a d-wave superconductor. The pair breaking is weaker for hole dopants, which induce magnetic moments, than for electron dopants. Furthermore, both Pt and Sn doping have a similar effect on superconductivity despite being on different dopant sites, arguing against the notion that superconductivity lives predominantly in the CeIn(3) planes of these materials. In addition, we shed qualitative understanding on the doping dependence with density functional theory calculations.

Sequential spin polarization of the Fermi surface pockets in URu2Si2 and its implications for the hidden order.

Using Shubnikov-de Haas oscillations measured in URu2Si2 over a broad range in a magnetic field of 11-45 T, we find a cascade of field-induced Fermi surface changes within the hidden order phase I and further signatures of oscillations within field-induced phases III and V [previously discovered by Kim et al., [Phys. Rev. Lett. 91, 256401 (2003)]. A comparison of kinetic and Zeeman energies indicates a pocket-by-pocket polarization of the Fermi surface leading up to the destruction of the hidden order phase I at ≈35 T. The anisotropy of the Zeeman energy driving the transitions in URu2Si2 points to an itinerant hidden order parameter involving quasiparticles whose spin degrees of freedom depart significantly from those of free electrons.

Anisotropic critical magnetic fluctuations in the ferromagnetic superconductor UCoGe.

We report neutron scattering measurements of critical magnetic excitations in the weakly ferromagnetic superconductor UCoGe. The strong non-Landau damping of the excitations we observe, although unusual, has been found in another related ferromagnet, UGe(2) at zero pressure. However, we also find that there is a significant anisotropy of the magnetic correlation length in UCoGe that contrasts with an almost isotropic length for UGe(2). The values of the magnetic correlation length and damping are found to be compatible with superconductivity on small Fermi-surface pockets. The anisotropy may be important to explain why UCoGe is a superconductor at zero pressure while UGe(2) is not.

Phase stabilization by electronic entropy in plutonium.

Plutonium metal undergoes an anomalously large 25% collapse in volume from its largest volume δ phase (δ-Pu) to its low temperature α phase, yet the underlying thermodynamic mechanism has largely remained a mystery. Here we use magnetostriction measurements to isolate a previously hidden yet substantial electronic contribution to the entropy of δ-Pu, which we show to be crucial for the stabilization of this phase. The entropy originates from two competing instabilities of the 5f-electron shell, which we show to drive the volume of Pu in opposing directions, depending on the temperature and volume. Using calorimetry measurements, we establish a robust thermodynamic connection between the two excitation energies, the atomic volume, and the previously reported excess entropy of δ-Pu at elevated temperatures.

Weak itinerant antiferromagnetism in PuIn3 explored using 115In nuclear quadrupole resonance.

The results of (115)In nuclear quadrupole resonance (NQR) measurements on PuIn3 are reported. Three of the four NQR lines of (115)In expected for nuclear spin I = 9/2 are observed. The equal spacing of these lines at 20 K yields the NQR frequency of νQ = 10.45 MHz, and the asymmetry parameter of the electric field gradient η = 0. The NQR line profile and the nuclear spin-lattice relaxation rate 1/T1 display an abrupt change at 14 K, which is associated with the onset of long-range antiferromagnetic order. The temperature dependences of the staggered magnetization MQ(T), extracted from the NQR spectra, and 1/T1 below TN = 14 K are well explained by the self-consistent renormalization (SCR) theory for spin fluctuations. In addition, the scaling between T1T and MQ(T)/MQ(0) is also consistent with the predictions of SCR theory, providing further evidence that PuIn3 is a weak itinerant antiferromagnet in which spin fluctuations around the antiferromagnetic wavevector play a major role in the system's behavior at finite temperatures.

Controllable chirality-induced geometrical Hall effect in a frustrated highly correlated metal.

A current of electrons traversing a landscape of localized spins possessing non-coplanar magnetic order gains a geometrical (Berry) phase, which can lead to a Hall voltage independent of the spin-orbit coupling within the material-a geometrical Hall effect. Here we show that the highly correlated metal UCu(5) possesses an unusually large controllable geometrical Hall effect at T<1.2 K due to its frustration-induced magnetic order. The magnitude of the Hall response exceeds 20% of the ν=1 quantum Hall effect per atomic layer, which translates into an effective magnetic field of several hundred Tesla acting on the electrons. The existence of such a large geometric Hall response in UCu(5) opens a new field of enquiry into the importance of the role of frustration in highly correlated electron materials.

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.

Magnetic order in Pu2M3Si5 (M = Co, Ni).

The physical properties including magnetic susceptibility, specific heat, and electrical resistivity of two new plutonium compounds Pu2M3Si5 (M = Co, Ni) are reported. Pu2Ni3Si5 crystallizes in the orthorhombic U2Co3Si5 structure type, which can be considered a variant of the BaAl4 tetragonal structure, while Pu2Co3Si5 adopts the closely related monoclinic Lu2Co3Si5 type. Magnetic order is observed in both compounds, with Pu2Ni3Si5 ordering ferromagnetically at T(C) = 65 K then undergoing a transition into an antiferromagnetic state below T(N) = 35 K. Two successive magnetic transitions are also observed at T(mag1) = 38 K and T(mag2) = 5 K in Pu2Co3Si5. Specific heat measurements reveal that these two materials have a moderately enhanced Sommerfeld coefficient γ ∼ 100 mJ/mol Pu K(2) in the magnetic state with comparable RKKY and Kondo energy scales.

Synthesis, structure and physical properties of YbNi3Al9.23.

The physical properties of YbNi(3)Al(9.23(1)), including the crystal structure, magnetization, specific heat, valence, and electrical resistivity, are reported. Single crystal x-ray diffraction reveals that the compound crystallizes with the rhombohedral space group R32 and has unit cell parameters a = 7.2443(3) Å and c = 27.251(3) Å with some crystallographic disorder at Al sites. The compound orders antiferromagnetically at T(N) = 3 K despite the presence of strong ferromagnetic correlations, accompanied by a spin-flop-like transition to a moment-aligned state above 0.1 T. X-ray absorption spectroscopy and magnetic susceptibility measurements indicate a localized Yb(3+) electronic configuration, while the Sommerfeld coefficient for the magnetically ordered state was determined as approximately 135 mJ mol(-1) K(-2), suggesting moderately heavy fermion behavior. Therefore, these data indicate a balance between competing Ruderman-Kittel-Kasuya-Yosida (RKKY) and Kondo interactions in YbNi(3)Al(9.23(1)) with a somewhat dominant RKKY interaction that leads to a relatively high ordering temperature.