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.

Isotropic quantum scattering and unconventional superconductivity.

Superconductivity without phonons has been proposed for strongly correlated electron materials that are tuned close to a zero-temperature magnetic instability of itinerant charge carriers. Near this boundary, quantum fluctuations of magnetic degrees of freedom assume the role of phonons in conventional superconductors, creating an attractive interaction that 'glues' electrons into superconducting pairs. Here we show that superconductivity can arise from a very different spectrum of fluctuations associated with a local (or Kondo-breakdown) quantum critical point that is revealed in isotropic scattering of charge carriers and a sublinear, temperature-dependent electrical resistivity. At this critical point, accessed by applying pressure to the strongly correlated, local-moment antiferromagnet CeRhIn(5), magnetic and charge fluctuations coexist and produce electronic scattering that is maximal at the optimal pressure for superconductivity. This previously unanticipated source of pairing glue opens possibilities for understanding and discovering new unconventional forms of superconductivity.

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.

Vortex lattice studies in CeCoIn5 with H is orthogonal to c.

We present small angle neutron scattering studies of the vortex lattice (VL) in CeCoIn5 with magnetic fields applied parallel (H) to the antinodal [100] and nodal [110] directions. For H is parallel to [100], a single VL orientation is observed, while a 90° reorientation transition is found for H is parallel to [110]. For both field orientations and VL configurations we find a distorted hexagonal VL with an anisotropy, Γ=2.0±0.05. The VL form factor shows strong Pauli paramagnetic effects similar to what have previously been reported for H is parallel to [001]. At high fields, above which the upper critical field (H(c2)) becomes a first-order transition, an increased disordering of the VL is observed.

Hidden magnetism and quantum criticality in the heavy fermion superconductor CeRhIn5.

With only a few exceptions that are well understood, conventional superconductivity does not coexist with long-range magnetic order (for example, ref. 1). Unconventional superconductivity, on the other hand, develops near a phase boundary separating magnetically ordered and magnetically disordered phases. A maximum in the superconducting transition temperature T(c) develops where this boundary extrapolates to zero Kelvin, suggesting that fluctuations associated with this magnetic quantum-critical point are essential for unconventional superconductivity. Invariably, though, unconventional superconductivity masks the magnetic phase boundary when T < T(c), preventing proof of a magnetic quantum-critical point. Here we report specific-heat measurements of the pressure-tuned unconventional superconductor CeRhIn5 in which we find a line of quantum-phase transitions induced inside the superconducting state by an applied magnetic field. This quantum-critical line separates a phase of coexisting antiferromagnetism and superconductivity from a purely unconventional superconducting phase, and terminates at a quantum tetracritical point where the magnetic field completely suppresses superconductivity. The T --> 0 K magnetic field-pressure phase diagram of CeRhIn5 is well described with a theoretical model developed to explain field-induced magnetism in the high-T(c) copper oxides, but in which a clear delineation of quantum-phase boundaries has not been possible. These experiments establish a common relationship among hidden magnetism, quantum criticality and unconventional superconductivity in copper oxides and heavy-electron systems such as CeRhIn5.

Unconventional superconductivity in PuCoGa5.

In the Bardeen-Cooper-Schrieffer theory of superconductivity, electrons form (Cooper) pairs through an interaction mediated by vibrations in the underlying crystal structure. Like lattice vibrations, antiferromagnetic fluctuations can also produce an attractive interaction creating Cooper pairs, though with spin and angular momentum properties different from those of conventional superconductors. Such interactions have been implicated for two disparate classes of materials--the copper oxides and a set of Ce- and U-based compounds. But because their transition temperatures differ by nearly two orders of magnitude, this raises the question of whether a common pairing mechanism applies. PuCoGa5 has a transition temperature intermediate between those classes and therefore may bridge these extremes. Here we report measurements of the nuclear spin-lattice relaxation rate and Knight shift in PuCoGa5, which demonstrate that it is an unconventional superconductor with properties as expected for antiferromagnetically mediated superconductivity. Scaling of the relaxation rates among all of these materials (a feature not exhibited by their Knight shifts) establishes antiferromagnetic fluctuations as a likely mechanism for their unconventional superconductivity and suggests that related classes of exotic superconductors may yet be discovered.

Electronic duality in strongly correlated matter.

Superconductivity develops from an attractive interaction between itinerant electrons that creates electron pairs, which condense into a macroscopic quantum state-the superconducting state. On the other hand, magnetic order in a metal arises from electrons localized close to the ionic core and whose interaction is mediated by itinerant electrons. The dichotomy between local moment magnetic order and superconductivity raises the question of whether these two states can coexist and involve the same electrons. Here, we show that the single 4f electron of cerium in CeRhIn(5) simultaneously produces magnetism, characteristic of localization, and superconductivity that requires itinerancy. The dual nature of the 4f-electron allows microscopic coexistence of antiferromagnetic order and superconductivity whose competition is tuned by small changes in pressure and magnetic field. Electronic duality contrasts with conventional interpretations of coexisting spin-density magnetism and superconductivity and offers a new avenue for understanding complex states in classes of materials.

Hybridization and superconducting gaps in the heavy-fermion superconductor PuCoGa5 probed via the dynamics of photoinduced quasiparticles.

We have examined the relaxation of photoinduced quasiparticles in the heavy-fermion superconductor PuCoGa5. The deduced electron-phonon coupling constant is incompatible with the measured superconducting transition temperature Tc=18.5 K, which speaks against phonon-mediated superconductivity. Upon lowering the temperature, we observe an order-of-magnitude increase of the quasiparticle relaxation time in agreement with the phonon bottleneck scenario--evidence for a hybridization gap in the electronic density of states. The modification of photoinduced reflectance in the superconducting state is consistent with the heavy character of the quasiparticles that participate in Cooper pairing.

Superconducting quantum critical point in CeCoIn(5-x)Sn(x).

We report a combined pressure-doping study in the nearly two-dimensional heavy fermion superconductor CeCoIn5 as its superconducting phase is driven to the normal state by Sn doping and/or applied pressure. Temperature-pressure-dependent electrical resistivity measurements were performed at the vicinity of a superconducting quantum critical point where Tc→0. A universal plot of the concentration- and pressure-dependent phase diagram suggests that for the concentrations studied a single mechanism is responsible for reducing Tc and bringing the system to the superconducting quantum critical point. A two-band model with hybridization controlled by pressure and doping provides a consistent description of the phase diagram and the suppression of the d-wave superconductivity in this material.

Evidence for a magnetically driven superconducting Q phase of CeCoIn5.

We have studied the magnetic order inside the superconducting phase of CeCoIn5 for fields along the [1 0 0] crystallographic direction using neutron diffraction. We find a spin-density wave order with an incommensurate modulation Q=(q,q,1/2) and q=0.45(1), which within our experimental uncertainty is indistinguishable from the spin-density wave found for fields applied along [1 -1 0]. The magnetic order is thus modulated along the lines of nodes of the d{x{2}-y{2}} superconducting order parameter, suggesting that it is driven by the electron nesting along the superconducting line nodes. We postulate that the onset of magnetic order leads to reconstruction of the superconducting gap function and a magnetically induced pair density wave.

High-temperature weak ferromagnetism in a low-density free-electron gas.

The magnetic properties of the ground state of a low-density free-electron gas in three dimensions have been the subject of theoretical speculation and controversy for seven decades. Not only is this a difficult theoretical problem to solve, it is also a problem which has not hitherto been directly addressed experimentally. Here we report measurements on electron-doped calcium hexaboride (CaB6) which, we argue, show that-at a density of 7× 1019 electrons cm-3-the ground state is ferromagnetically polarized with a saturation moment of 0.07 µB per electron. Surprisingly, the magnetic ordering temperature of this itinerant ferromagnet is 600 K, of the order of the Fermi temperature of the electron gas.

Field-induced coupled superconductivity and spin density wave order in the heavy fermion compound CeCoIn5.

The high-field superconducting state in CeCoIn(5) has been studied by transverse field muon spin rotation measurements with an applied field parallel to the crystallographic c axis close to the upper critical field mu(0)H(c2) = 4.97 T. At magnetic fields mu(0)H > or = 4.8 T the muon Knight shift is enhanced and the superconducting transition changes from second order towards first order as predicted for Pauli-limited superconductors. The field and temperature dependence of the transverse muon spin relaxation rate sigma reveal paramagnetic spin fluctuations in the field regime from 2 T < or = mu(0)H < 4.8 T. In the normal state close to H(c2) correlated spin fluctuations as described by the self-consistent renormalization theory are observed. The results support the formation of a mode-coupled superconducting and antiferromagnetically ordered phase in CeCoIn(5) for H directed parallel to the c axis.

Itinerant spin excitations near the hidden order transition in URu(2)Si(2).

By means of neutron scattering we show that the high temperature precursor to the hidden order state of the heavy fermion superconductor URu(2)Si(2) exhibits heavily damped incommensurate paramagnons whose strong energy dispersion is very similar to that of the long-lived longitudinal f spin excitations that appear below T(0). This suggests that there is a strongly hybridized character to the itinerant excitations observed previously above the hidden order transition. Here we present evidence that the itinerant excitations, like those in chromium, are due to Fermi surface nesting of hole and electron pockets; hence the hidden order phase probably originates from a Fermi surface instability. We identify wavevectors that span nested regions of a f-d hybridized band calculation and that match the neutron spin crossover from incommensurate to commensurate on approach to the hidden order phase.

Unusual diffusive effects on the ESR of Nd³âº ions in the tunable topologically nontrivial semimetal YBiPt.

Electron spin resonance (ESR) of diluted Nd(3+) ions in the topologically nontrivial semimetallic (TNSM) YBiPt compound is reported. The cubic YBiPt compound is a non-centrosymmetric half Heusler material which crystallizes in the F43m space group. The low temperature Nd(3+) ESR spectra showed a g-value of 2.66(4) corresponding to a Γ6 cubic crystal field Kramers' doublet ground state. Remarkably, the observed metallic and diffusive (Dysonian) Nd(3+) lineshape presented an unusual dependence with grain size, microwave power, Nd(3+) concentration and temperature. Moreover, the spin dynamic of the localized Nd(3+) ions in YBiPt was found to be characteristic of a phonon-bottleneck regime. It is claimed that, in this regime for YBiPt, phonons are responsible for mediating the diffusion of the microwave energy absorbed at resonance by the Nd(3+) ions to the thermal bath throughout the skin depth (δ ≃ µm). We argue that this is only possible because of the existence of highly mobile conduction electrons inside the skin depth of YBiPt that are strongly coupled to the phonons by spin-orbit coupling. Therefore, our unexpected ESR results point to a coexistence of metallic and insulating behaviors within the skin depth of YBiPt. This scenario is discussed in the light of the TNSM properties of this compound.

X-ray photoemission study of CeTIn(5) (T = Co, Rh, Ir).

We investigated CeTIn5 (T = Co, Rh, Ir) using temperature- and angle-dependent x-ray photoemission spectroscopy. The Ce 3d core level has a very similar shape for all three materials and is indicative of weak f-hybridization. The spectra were analyzed using a simplified version of the Anderson impurity model, which yields a Ce 4f occupancy that is larger than 0.9. The temperature dependence shows a continuous, irreversible and exclusive broadening of the Ce 3d peaks, due to oxidation of Ce at the surface.

Nodal quasiparticle dynamics in the heavy fermion superconductor CeCoIn5 revealed by precision microwave spectroscopy.

CeCoIn5 is a heavy fermion superconductor with strong similarities to the high-Tc cuprates, including quasi-two-dimensionality, proximity to antiferromagnetism and probable d-wave pairing arising from a non-Fermi-liquid normal state. Experiments allowing detailed comparisons of their electronic properties are of particular interest, but in most cases are difficult to realize, due to their very different transition temperatures. Here we use low-temperature microwave spectroscopy to study the charge dynamics of the CeCoIn5 superconducting state. The similarities to cuprates, in particular to ultra-clean YBa2Cu3O(y), are striking: the frequency and temperature dependence of the quasiparticle conductivity are instantly recognizable, a consequence of rapid suppression of quasiparticle scattering below T(c); and penetration-depth data, when properly treated, reveal a clean, linear temperature dependence of the quasiparticle contribution to superfluid density. The measurements also expose key differences, including prominent multiband effects and a temperature-dependent renormalization of the quasiparticle mass.

Unconventional quantum criticality in the pressure-induced heavy-fermion superconductor CeRhIn5.

The lack of superconductivity in several candidate materials that exhibit a non-spin density wave quantum critical point has raised the question of whether the associated spectra of quantum fluctuations are beneficial to forming superconducting electron pairs. Here we discuss the possibility that the prototypical heavy-fermion antiferromagnet CeRhIn5 may be the first example of unconventional superconductors where superconductivity arises from Kondo-breakdown quantum criticality.

Dimensional crossover of quantum critical behavior in CeCoIn5.

The nature of quantum criticality in CeCoIn5 is studied by low-temperature thermal expansion alpha(T). At the field-induced quantum critical point at H = 5 T a crossover scale T* approximately 0.3 K is observed, separating alpha(T)/T proportional, variant T(-1) from a weaker T(-1/2) divergence. We ascribe this change to a crossover in the dimensionality of the critical fluctuations which may be coupled to a change from unconventional to conventional quantum criticality. Disorder, whose effect on quantum criticality is studied in CeCoIn(5-x)Sn(x) (0 < or = x < or = 0.18), shifts T* towards higher temperatures.

Precursor State to Unconventional Superconductivity in CeIrIn5.

We present Hall effect and magnetoresistance measurements in the heavy fermion superconductor CeIrIn(5). At low temperature, a Kondo coherent state is established. Deviations from Kohler's rule and a quadratic temperature dependence of the cotangent of the Hall angle are reminiscent of properties observed in the high-temperature superconducting cuprates. A striking observation pertains to the presence of a precursor state--characterized by a change in the Hall mobility--that precedes the superconductivity in this material, in similarity to the pseudogap in the cuprate superconductors.

Andreev reflection in heavy-fermion superconductors and order parameter symmetry in CeCoIn5.

Differential conductance spectra are obtained from nanoscale junctions on the heavy-fermion superconductor CeCoIn5 along three major crystallographic orientations. Consistency and reproducibility of characteristic features among the junctions ensure their spectroscopic nature. All junctions show a similar conductance asymmetry and Andreev reflectionlike conductance with a reduced signal ( approximately 10%-13%), both commonly observed in heavy-fermion superconductor junctions. Analysis using the extended Blonder-Tinkham-Klapwijk model indicates that our data provide the first spectroscopic evidence for d_{x;{2}-y;{2}} symmetry. To quantify our conductance spectra, we propose a model by considering the general phenomenology in heavy fermions, the two-fluid behavior, and an energy-dependent density of states. Our model fits to the experimental data remarkably well and should invigorate further investigations.