Search

The electronic structure of plutonium metal and its compounds pose a grand challenge for a fundamental understanding of the Pu-5$f$ electron character. For 30 years the plutonium chalcogenides have been especially challenging, and multiple theoretical scenarios have been proposed to explain their unusual behavior. We present extensive high-resolution photoemission data on a single crystal of PuTe, which has also been proposed as a topological insulator. The new experimental results on this mixed-valent material provide a constraint to the theoretical modeling and new dynamical mean-field theory calculations agree with the experimental results. Comparisons with Pu metal provide new insight in understanding its complex electronic structure., Comment: 5 pages with 4 eps figures embedded, supplementary material

We present the results of high-resolution valence-band photoemission spectroscopic study of SmB6 which shows evidence for a V-shaped density of states of surface origin within the bulk gap. The spectroscopy data is interpreted in terms of the existence of heavy 4f surface states, which may be useful in resolving the controversy concerning the disparate surface Fermi-surface velocities observed in experiments. Most importantly, we find that the temperature dependence of the valence-band spectrum indicates that a small feature appears at a binding energy of about -9 meV at low temperatures. We attribute this feature to a resonance caused by the spin-exciton scattering in SmB6 which destroys the protection of surface states due to time-reversal invariance and spin-momentum locking. The existence of a low-energy spin-exciton may be responsible for the scattering which suppresses the formation of coherent surface quasi-particles and the appearance of the saturation of the resistivity to temperatures much lower than the coherence temperature associated with the opening of the bulk gap.

We present measurements of the thermoelectric power of the plutonium-based unconventional superconductor PuCoGa$_{5}$. The data is interpreted within a phenomenological model for the quasiparticle density of states of intermediate valence systems and the results are compared with results obtained from photoemission spectroscopy. The results are consistent with intermediate valence nature of 5$f$-electrons, furthermore, we propose that measurements of the Seebeck coefficient can be used as a probe of density of states in this material, thereby providing a link between transport measurements and photoemission in strongly correlated materials. We discuss these results and their implications for the electronic structure determination of other strongly correlated systems, especially actinide materials., Comment: Accepted for publication in Phys. Rev. B (October 24, 2016)

The low-temperature microscopic magnetic properties of the quasi-2D heavyfermion compound, CePt2In7 are investigated by using a positive muon-spin rotation and relaxation (?muSR) technique. Clear evidence for the formation of a commensurate antiferromagnetic order below TN=5.40 K is presented. The magnetic order parameter is shown to fit well to a modified BSC gap-energy function in a strong-coupling scenario., Comment: Accepted in Journal of Physics: Conference Series (2014)

Fermi-surface topology governs the relationship between magnetism and superconductivity in iron-based materials. Using low-temperature transport, angle-resolved photoemission, and x-ray diffraction we show unambiguous evidence of large Fermi surface reconstruction in CaFe$_{2}$As$_{2}$ at magnetic spin-density-wave and nonmagnetic collapsed-tetragonal ($cT$) transitions. For the $cT$ transition, the change in the Fermi surface topology has a different character with no contribution from the hole part of the Fermi surface. In addition, the results suggest that the pressure effect in CaFe$_{2}$As$_{2}$ is mainly leading to a rigid-band-like change of the valence electronic structure. We discuss these results and their implications for magnetism and superconductivity in this material., Comment: Accepted for publication in Phys. Rev. Lett. (April 3, 2014)

Possible topological nature of Kondo and mixed valence insulators has been a recent topic of interest in condensed matter physics. Attention has focused on SmB6, which has long been known to exhibit low temperature transport anomaly, whose origin is of independent interest. We argue that it is possible to resolve the topological nature of surface states by uniquely accessing the surface electronic structure of the low temperature anomalous transport regime through combining state-of-the-art laser- and synchrotron-based angle-resolved photoemission spectroscopy (ARPES) with or without spin resolution. A combination of low temperature and ultra-high resolution (laser) which is lacking in previous ARPES studies of this compound is the key to resolve the possible existence of topological surface state in SmB6. Here we outline an experimental algorithm to systematically explore the topological versus trivial or mixed (topological and trivial surface state admixture as in the first 3D TI Bi$_{1-x}$Sb$_x$) nature of the surface states in Kondo and mixed valence insulators. We conclude based on this methodology that the observed topology of the surface Fermi surface in our low temperature data considered within the level of current resolution is consistent with the theoretically predicted topological picture, suggesting a topological origin of the dominant in-gap ARPES signal in SmB6.}, Comment: 15 pages, 6 Figures, Submitted June'13; Published as SI in Nature Commun. 4, 2991 (2013)

The advent of Dirac materials has made it possible to realize two dimensional gases of relativistic fermions with unprecedented transport properties in condensed matter. Their photoconductive control with ultrafast light pulses is opening new perspectives for the transmission of current and information. Here we show that the interplay of surface and bulk transient carrier dynamics in a photoexcited topological insulator can control an essential parameter for photoconductivity - the balance between excess electrons and holes in the Dirac cone. This can result in a strongly out of equilibrium gas of hot relativistic fermions, characterized by a surprisingly long lifetime of more than 50 ps, and a simultaneous transient shift of chemical potential by as much as 100 meV. The unique properties of this transient Dirac cone make it possible to tune with ultrafast light pulses a relativistic nanoscale Schottky barrier, in a way that is impossible with conventional optoelectronic materials., Comment: Nature Communications, in press (12 pages, 6 figures)

Using circular dichroism-angle resolved photoemission spectroscopy (CD-ARPES), we report a study of the effect of angular momentum transfer between polarized photons and topological surface states on the surface of highly bulk insulating topological insulator Bi2Te2Se. The photoelectron dichroism is found to be strongly modulated by the frequency of the helical photons including a dramatic sign-flip. Our results suggest that the observed dichroism and its sign-flip are consequences of strong coupling between the photon field and the spin-orbit nature of the Dirac modes on the surface. Our studies reveal the intrinsic dichroic behavior of topological surface states and point toward the potential utility of bulk insulating topological insulators in device applications., Comment: 5 pages, 4 figures

The Kondo insulator SmB6 has long been known to exhibit low temperature (T < 10K) transport anomaly and has recently attracted attention as a new topological insulator candidate. By combining low-temperature and high energy-momentum resolution of the laser-based ARPES technique, for the first time, we probe the surface electronic structure of the anomalous conductivity regime. We observe that the bulk bands exhibit a Kondo gap of 14 meV and identify in-gap low-lying states within a 4 meV window of the Fermi level on the (001)-surface of this material. The low-lying states are found to form electron-like Fermi surface pockets that enclose the X and the Gamma points of the surface Brillouin zone. These states disappear as temperature is raised above 15K in correspondence with the complete disappearance of the 2D conductivity channels in SmB6. While the topological nature of the in-gap metallic states cannot be ascertained without spin (spin-texture) measurements our bulk and surface measurements carried out in the transport-anomaly-temperature regime (T < 10K) are consistent with the first-principle predicted Fermi surface behavior of a topological Kondo insulator phase in this material., Comment: 4 Figures, 6 Pages

Ultrafast optical spectroscopy is used to study the antiferromagnetic f-electron system USb2. We observe the opening of two charge gaps at low temperatures (<45 K), arising from renormalization of the electronic structure. Analysis of our data indicates that one gap is due to hybridization between localized f-electron and conduction electron bands, while band renormalization involving magnons leads to the emergence of the second gap. These experiments thus enable us to shed light on the complex electronic structure emerging at the Fermi surface in f-electron systems.

We study, using high-resolution angle-resolved photoemission spectroscopy, the evolution of the electronic structure in URu2Si2 at the Gamma, Z and X high-symmetry points from the high-temperature Kondo-screened regime to the low-temperature `hidden-order' (HO) state. At all temperatures and symmetry points, we find structures resulting from the interaction between heavy and light bands, related to the Kondo lattice formation. At the X point, we directly measure a hybridization gap of 11 meV already open at temperatures above the ordered phase. Strikingly, we find that while the HO induces pronounced changes at Gamma and Z, the hybridization gap at X does not change, indicating that the hidden-order parameter is anisotropic. Furthermore, at the Gamma and Z points, we observe the opening of a gap in momentum in the HO state, and show that the associated electronic structure results from the hybridization of a light electron band with the Kondo-lattice bands characterizing the paramagnetic state., Comment: Updated published version. Mansucript + Supplemental Material (8 pages, 9 figures). Submitted 16 September 2012

We report extensive measurements on a new compound (Yb0.24Sn0.76)Ru that crystallizes in the cubic CsCl structure. Valence band photoemission and L3 x-ray absorption show no divalent component in the 4f configuration of Yb. Inelastic neutron scattering (INS) indicates that the eight-fold degenerate J-multiplet of Yb3+ is split by the crystalline electric field (CEF) into a {\Gamma}7 doublet ground state and a {\Gamma}8 quartet at an excitation energy 20 meV. The magnetic susceptibility can be fit very well by this CEF scheme under the assumption that a {\Gamma}6 excited state resides at 32 meV; however, the {\Gamma}8/{\Gamma}6 transition expected at 12 meV was not observed in the INS. The resistivity follows a Bloch- Gr\"uneisen law shunted by a parallel resistor, as is typical of systems subject to phonon scattering with no apparent magnetic scattering. All of these properties can be understood as representing simple local moment behavior of the trivalent Yb ion. At 1 K, there is a peak in specific heat that is too broad to represent a magnetic phase transition, consistent with absence of magnetic reflections in neutron diffraction. On the other hand, this peak also is too narrow to represent the Kondo effect in the {\Gamma}7 ground state doublet. On the basis of the field-dependence of the specific heat, we argue that antiferromagnetic shortrange order (possibly co-existing with Kondo physics) occurs at low temperatures. The long-range magnetic order is suppressed because the Yb site occupancy is below the percolation threshold for this disordered compound.

We present an angle-resolved photoemission spectroscopy study of the electronic structure of SnTe, and compare the experimental results to ab initio band structure calculations as well as a simplified tight-binding model of the p-bands. Our study reveals the conjectured complex Fermi surface structure near the L-points showing topological changes in the bands from disconnected pockets, to open tubes, and then to cuboids as the binding energy increases, resolving lingering issues about the electronic structure. The chemical potential at the crystal surface is found to be 0.5eV below the gap, corresponding to a carrier density of p =1.14x10^{21} cm^{-3} or 7.2x10^{-2} holes per unit cell. At a temperature below the cubic-rhombohedral structural transition a small shift in spectral energy of the valance band is found, in agreement with model predictions., Comment: 4 figures

We report a comprehensive electronic structure investigation of the paramagnetic (PM), the large moment antiferromagnetic (LMAF), and the hidden order (HO) phases of URu$_2$Si$_2$. We have performed relativistic full-potential calculations on the basis of the density functional theory (DFT), employing different exchange-correlation functionals to treat electron correlations within the open $5f$-shell of uranium. Specifically, we investigate---through a comparison between calculated and low-temperature experimental properties---whether the $5f$ electrons are localized or delocalized in URu$_2$Si$_2$. We also performed dynamical mean field theory calculations (LDA+DMFT) to investigate the temperature evolution of the quasi-particle states at 100~K and above, unveiling a progressive opening of a quasi-particle gap at the chemical potential when temperature is reduced. A detailed comparison of calculated properties with known experimental data demonstrates that the LSDA and GGA approaches, in which the uranium $5f$ electrons are treated as itinerant, provide an excellent explanation of the available low-temperature experimental data of the PM and LMAF phases. We show furthermore that due to a materials-specific Fermi surface instability a large, but partial, Fermi surface gapping of up to 750 K occurs upon antiferromagnetic symmetry breaking. The occurrence of the HO phase is explained through dynamical symmetry breaking induced by a mode of long-lived antiferromagnetic spin-fluctuations. This dynamical symmetry breaking model explains why the Fermi surface gapping in the HO phase is similar but smaller than that in the LMAF phase and it also explains why the HO and LMAF phases have the same Fermi surfaces yet different order parameters. Suitable derived order parameters for the HO are proposed to be the Fermi surface gap or the dynamic spin-spin correlation function., Comment: 23 pages, 20 figures

We report the properties of two new isostructural compounds, U3Bi4Ni3 and U3Bi4Rh3. The first of these compounds is non-metallic, and the second is a nearly ferromagnetic metal, both as anticipated from their electron count relative to other U-based members of the larger 3-4-3 family. For U3Bi4Rh3, a logarithmic increase of C/T below 3 K, a resistivity proportional to T^4/3, and the recovery of Fermi-liquid behavior in both properties with applied fields greater than 3T, suggest that U3Bi4Rh3 may be a new example of a material displaying ferromagnetic quantum criticality., Comment: 24 pages, 7 figures, submitted to Physical Review B

By combining the local density approximation (LDA) with dynamical mean field theory (DMFT), we report a systematic analysis of the spectral properties of $\delta$-plutonium with varying $5f$ occupancy. The LDA Hamiltonian is extracted from a tight-binding (TB) fit to full-potential linearized augmented plane-wave (FP-LAPW) calculations. The DMFT equations are solved by the exact quantum Monte Carlo (QMC) method and the Hubbard-I approximation. We have shown for the first time the strong sensitivity of the spectral properties to the $5f$ occupancy, which suggests using this occupancy as a fitting parameter in addition to the Hubbard $U$. By comparing with PES data, we conclude that the ``open shell'' $5f^{5}$ configuration gives the best agreement, resolving the controversy over $5f$ ``open shell'' versus ``close shell'' atomic configurations in $\delta$-Pu., Comment: 6 pages, 2 embedded color figures, to appear in Physical Review B

Ultrafast time-resolved photoinduced reflectivity is measured for the itinerant antiferromagnet UNiGa$_{5}$ ($T_{N} \approx$85 K) from room temperature to 10 K. The relaxation time $\tau$ shows a sharp increase at $T_{N}$ consistent with the opening of a spin gap. In addition, the temperature dependence of $\tau$ below $T_{N}$ is consistent with the opening of a spin gap leading to a quasiparticle recombination bottleneck as revealed by the Rothwarf-Taylor model. This contrasts with canonical heavy fermions such as CeCoIn$_{5}$ where the recombination bottleneck arises from the hybridization gap., Comment: 5 pages, 5 figures

The electronic structure of the first Pu based superconductor PuCoGa5 is explored using photoelectron spectroscopy and a novel theoretical scheme. Exceptional agreement between calculation and experiment defines a path forward for understanding electronic structure aspects of Pu based materials. The photoemission results show two separate regions of 5f electron spectral intensity, one at the Fermi energy and another centered 1.2 eV below the Fermi level. The results for PuCoGa5 clearly indicate 5f electron behavior on the threshold between localized and itinerant. Comparisons to delta phase Pu metal show a broader framework for understanding the fundamental electronic properties of the Pu 5f levels in general within two configurations, one localized and one itinerant., Comment: accepted by PRL

Single crystal antiferromagnetic USb2 was studied at 15K by angle-resolved photoemission with an overall energy resolution of 24 meV. The measurements unambiguously show the dispersion of extremely narrow bands situated near the Fermi level. The peak at the Fermi level represents the narrowest feature observed in 5f-electron photoemission to date. The natural linewidth of the feature just below the Fermi level is not greater than 10 meV. Normal emission data indicate a three dimensional aspect to the electronic structure of this layered material., Comment: 22 pages including figures

We present a theoretical model of the electronic structure of delta-Pu that is consistent with many of the electronic structure related properties of this complex metal. In particular we show that the theory is capable of reproducing the valence band photoelectron spectrum of delta-Pu. We report new experimental photoelectron spectra at several photon energies and present evidence that the electronic structure of delta-Pu is unique among the elements, involving a 5f shell with four 5f electrons in a localized multiplet, hybridizing with valence states, and approximately one 5f electron forming a completely delocalized band state., Comment: 4 pages, 1 figure