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C. H. Booth

Publications and source records attributed to C. H. Booth.

At least 19 recordsLinked to original sources

Kondo quasiparticle dynamics observed by resonant inelastic x-ray scattering

Effective models focused on pertinent low-energy degrees of freedom have substantially contributed to our qualitative understanding of quantum materials. An iconic example, the Kondo model, was key to demonstrating that the rich phase diagrams of correlated metals originate from the interplay of localized and itinerant electrons. Modern electronic structure calculations suggest that to achieve quantitative material-specific models, accurate consideration of the crystal field and spin-orbit interactions is imperative. This poses the question of how local high-energy degrees of freedom become incorporated into a collective electronic state. Here, we use resonant inelastic x-ray scattering (RIXS) on CePd$_3$ to clarify the fate of all relevant energy scales. We find that even spin-orbit excited states acquire pronounced momentum-dependence at low temperature - the telltale sign of hybridization with the underlying metallic state. Our results demonstrate how localized electronic degrees of freedom endow correlated metals with new properties, which is critical for a microscopic understanding of superconducting, electronic nematic, and topological states.

cond-mat.str-el

Probing 5f-state configurations in URu2Si2 with U L3-edge resonant x-ray emission spectroscopy

Resonant x-ray emission spectroscopy (RXES) was employed at the U L3 absorption edge and the La1 emission line to explore the 5f occupancy, nf, and the degree of 5f orbital delocalization in the hidden order compound URu2Si2. By comparing to suitable reference materials such as UF4, UCd11, and alpha-U, we conclude that the 5f orbital in URu2Si2 is at least partially delocalized with nf = 2.87 +/- 0.08, and does not change with temperature down to 10 K within the estimated error. These results place further constraints on theoretical explanations of the hidden order, especially those requiring a localized f2 ground state.

cond-mat.str-el

Isochronal annealing effects on local structure, crystalline fraction, and undamaged region size of radiation damage in Ga-stabilized $δ$-Pu

The effects on the local structure due to self-irradiation damage of Ga stabilized $δ$-Pu stored at cryogenic temperatures have been examined using extended x-ray absorption fine structure (EXAFS) experiments. Extensive damage, seen as a loss of local order, was evident after 72 days of storage below 15 K. The effect was observed from both the Pu and Ga sites, although less pronounced around Ga. Isochronal annealing was performed on this sample to study the annealing processes that occur between cryogenic and room temperature storage conditions, where damage is mostly reversed. Damage fractions at various points along the annealing curve have been determined using an amplitude-ratio method, standard EXAFS fitting, and a spherical crystallite model, and provide information complementary to previous electrical resistivity- and susceptibility-based isochronal annealing studies. The use of a spherical crystallite model accounts for the changes in EXAFS spectra using just two parameters, namely, the crystalline fraction and the particle radius. Together, these results are discussed in terms of changes to the local structure around Ga and Pu throughout the annealing process and highlight the unusual role of Ga in the behavior of the lowest temperature anneals.

cond-mat.mtrl-sci

The effects of Co3O4 on the Structure and Unusual Magnetism of LaCoO3

Bulk La_wCoO3 particles with w=1.1, 1.0, 0.9, 0.8, and 0.7 were synthesized using starting materials with varying molar ratios of La2O3 and Co3O4. The resulting particles are characterized as LaCoO3 crystals interfaced with a crystalline Co3O4 phase. X-ray and neutron scattering data show little effect on the average structure and lattice parameters of the LaCoO3 phase resulting from the Co3O4 content, but magnetization data indicate that the amount of Co3O4 strongly affects the ferromagnetic ordering at the interfaces below T_C ~89K. In addition to ferromagnetic long-range order, LaCoO3 exhibits antiferromagnetic behavior with an unusual temperature dependence. The magnetization for fields 20 Oe < H < 5 kOe is fit to a combination of a power law ((T-T_C)/T_C)^beta behavior representing the ferromagnetic long-range order and sigmoid-convoluted Curie-Weiss-like behavior representing the antiferromagnetic behavior. The critical exponent beta=0.63 +- 0.02 is consistent with 2D (surface) ordering. Increased Co3O4 correlates well to increased ferromagnetism. The weakening of the antiferromagnetism below T ~ 40K is a consequence of the lattice reaching a critical rhombahedral distortion as T is decreased for core regions far from the Co3O4 interfaces. We introduce a model that describes the ferromagnetic behavior of the interface regions and the unusual antiferromagnetism of the core regions.

cond-mat.str-el

The unusual magnetism of nanoparticle LaCoO3

Bulk and nanoparticle powders of LaCoO3 (LCO) were synthesized, and their magnetic and structural properties were studied using SQUID magnetometry and neutron diffraction. The bulk and large nanoparticles exhibit weak ferromagnetism (FM) below T ~ 85K and a crossover from strong to weak antiferromagnetic (AFM) correlations near a transition expressed in the lattice parameters, To ~ 40K. This crossover does not occur in the smallest nanoparticles; instead, the magnetic behavior is predominantly ferromagnetic. The amount of FM in the nanoparticles depends on the amount of Co3O4 impurity phase, which induces tensile strain on the LCO lattice. A core-interface model is introduced, with the core region exhibiting the AFM crossover and with FM in the interface region near surfaces and impurity phases.

cond-mat.str-el

Q-dependence of the spin fluctuations in the intermediate valence compound CePd3

We report inelastic neutron scattering experiments on a single crystal of the intermediate valence compound CePd3. At 300 K the magnetic scattering is quasielastic, with halfwidth of 23 meV, and is independent of momentum transfer Q. At low temperature, the Q-averaged magnetic spectrum is inelastic, exhibiting a broad peak centered near Emax = 55 meV. These results, together with the temperature dependence of the susceptibility, 4f occupation number, and specific heat, can be fit by the Kondo/Anderson impurity model. The low temperature scattering near Emax, however, shows significant variations with Q, reflecting the coherence of the 4f lattice. The intensity is maximal at (1/2, 1/2,0), intermediate at (1/2,0,0) and (0,0,0), and weak at (1/2,1/2,1/2). We discuss this Q-dependence in terms of current ideas about coherence in heavy fermion systems.

cond-mat.str-el

Magnetism in nanoparticle LaCoO3

LaCoO3 (LCO) nanoparticles were synthesized and their magnetic and structural properties were examined using SQUID magnetometery and neutron diffraction. The nanoparticles exhibit ferromagnetic long-range order beginning at T_C approximately 87K that persists to low temperatures. This behavior is contrasted with the ferromagnetism of bulk LCO, which also starts at T_C approximately 87K but is suppressed below a second transition at T_o approximately 37K, due to a structural phase transition. The ferromagnetism in both systems is attributed to the tensile stress from particle surfaces and impurity phase interfaces. This stress locally increases the Co-O-Co bond angle gamma, and competes with the thermal contraction of the lattice. It has recently been shown that LCO loses long-range ferromagnetic order when gamma decreases below the critical value gamma_c = 162.8 degrees. Consistent with this model, we show that gamma in nanoparticles remains larger than gamma_c at low temperatures, likely a consequence of all spins being in close proximity to surfaces or interfaces.

cond-mat.str-el

PuPt2In7: a computational and experimental investigation

Flux-grown single crystals of PuPt$_2$In$_7$ are characterized and found to be both non-superconducting and non-magnetic down to 2 K. The Sommerfeld specific heat coefficient of $\sim 250$ mJ/mol K$^2$ indicates heavy fermion behavior. We report the results of generalized gradient approximation (GGA)+$U$ calculations of PuPt$_2$In$_7$ and as yet unsynthesized isovalent PuPt$_2$Ga$_7$. The strength of the $c$-$f$ hybridization of PuPt$_2$In$_7$ is similar to the PuCoIn$_5$ superconductor. The bare and $f$-weighted susceptibility within the constant-matrix-element approximation is calculated, showing a maximum along the $q_z$ direction at $q_x = q_y = 0.5$. A similar and slightly stronger maximum is also found in the structurally related heavy-fermion materials PuCoGa$_5$ and PuCoIn$_5$. The absence of superconductivity in PuPt$_2$In$_7$ is examined based on the results of our calculations.

cond-mat.supr-con

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 (eg. 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 for understanding the strongly-correlated behavior of actinide materials.

cond-mat.str-el

Crystal fields, disorder, and antiferromagnetic short-range order in Yb0.24Sn0.76Ru

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 Γ7 doublet ground state and a Γ8 quartet at an excitation energy 20 meV. The magnetic susceptibility can be fit very well by this CEF scheme under the assumption that a Γ6 excited state resides at 32 meV; however, the Γ8/Γ6 transition expected at 12 meV was not observed in the INS. The resistivity follows a Bloch- Grüneisen 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 Γ7 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.

cond-mat.str-el

Electronic Structure of CeFeAsO1-xFx (x=0, 0.11/x=0.12) compounds

We report an extensive study on the intrinsic bulk electronic structure of the high-temperature superconductor CeFeAsO0.89F0.11 and its parent compound CeFeAsO by soft and hard x-ray photoemission, x-ray absorption and soft-x-ray emission spectroscopies. The complementary surface/bulk probing depth, and the elemental and chemical sensitivity of these techniques allows resolving the intrinsic electronic structure of each element and correlating it with the local structure, which has been probed by extended-x-ray absorption fine structure spectroscopy. The measurements indicate a predominant 4f1 (i.e. Ce3+) initial state configuration for Cerium and an effective valence-band-to-4f charge-transfer screening of the core hole. The spectra also reveal the presence of a small Ce f0 initial state configuration, which we assign to the occurrence of an intermediate valence state. The data reveal a reasonably good agreement with the partial density of states as obtained in standard density functional calculations over a large energy range. Implications for the electronic structure of these materials are discussed.

cond-mat.supr-con

Local structure and site occupancy of Cd and Hg substitutions in CeTIn5 (T=Co, Rh, Ir)

The CeTIn5 superconductors (T=Co, Rh, or Ir) have generated great interest due to their relatively Tc's, NFL behavior, and their proximity to AF order and quantum critical points. In contrast to small changes with the T-species, electron doping in CeT(In{1-x}Mx)5 with M=Sn and hole doping with Cd or Hg have a dramatic effect on the electronic properties at very low concentrations. The present work reports EXAFS measurements that address the substituent atom distribution as a function of T, M, and x, near the superconducting phase. Together with previous measurements for M=Sn, the proportion of the M atom residing on the In(1) site, f{In(1)}, increases in the order M=Cd, Sn, and Hg, ranging from about 40% to 70%, showing a strong preference for these substituents to occupy the In(1) site (random=20%). In addition, f{In(1)} ranges from 70% to 100% for M=Hg in the order T=Co, Rh, and Ir. These fractions track the changes in the atomic radii of the various species, and help explain the sharp dependence of Tc on substituting into the In site. However, it is difficult to reconcile the small concentrations of M with the dramatic changes in the ground state in the hole-doped materials with only an impurity scattering model. These results therefore indicate that while such substitutions have interesting local atomic structures with important electronic and magnetic consequences, other local changes in the electronic and magnetic structure are equally important in determining the bulk properties of these materials.

cond-mat.str-el

Local Structure of La1-xSrxCoO3 determined from EXAFS and neutron PDF studies

The combined local structure techniques, extended x-ray absorption fine structure (EXAFS) and neutron pair distribution function analysis, have been used for temperatures 4 <= T <= 330 K to rule out a large Jahn-Teller (JT) distortion of the Co-O bond in La1-xSrxCoO3 for a significant fraction of Co sites (x <= 0.35), indicating few, if any, JT-active, singly occupied e_g Co sites exist.

cond-mat.str-el

Quantifying structural damage from self-irradiation in a plutonium superconductor

The 18.5 K superconductor PuCoGa5 has many unusual properties, including those due to damage induced by self-irradiation. The superconducting transition temperature decreases sharply with time, suggesting a radiation-induced Frenkel defect concentration much larger than predicted by current radiation damage theories. Extended x-ray absorption fine-structure measurements demonstrate that while the local crystal structure in fresh material is well ordered, aged material is disordered much more strongly than expected from simple defects, consistent with strong disorder throughout the damage cascade region. These data highlight the potential impact of local lattice distortions relative to defects on the properties of irradiated materials and underscore the need for more atomic-resolution structural comparisons between radiation damage experiments and theory.

cond-mat.str-el

Ytterbium divalency and lattice disorder in near-zero thermal expansion YbGaGe

While near-zero thermal expansion (NZTE) in YbGaGe is sensitive to stoichiometry and defect concentration, the NZTE mechanism remains elusive. We present x-ray absorption spectra that show unequivocally that Yb is nearly divalent in YbGaGe and the valence does not change with temperature or with nominally 1% B or 5% C impurities, ruling out a valence-fluctuation mechanism. Moreover, substantial changes occur in the local structure around Yb with B and C inclusion. Together with inelastic neutron scattering measurements, these data indicate a strong tendency for the lattice to disorder, providing a possible explanation for NZTE in YbGaGe.

cond-mat.mtrl-sci

Self-contained Kondo effect in single molecules

Kondo coupling of f and conduction electrons is a common feature of f-electron intermetallics. Similar effects should occur in carbon ring systems(metallocenes). Evidence for Kondo coupling in Ce(C8H8)2 (cerocene) and the ytterbocene Cp*2Yb(bipy) is reported from magnetic susceptibility and L_III-edge x-ray absorption spectroscopy. These well-defined systems provide a new way to study the Kondo effect on the nanoscale, should generate insight into the Anderson Lattice problem, and indicate the importance of this often-ignored contribution to bonding in organometallics.

cond-mat.str-el

Anisotropic intermediate valence in Yb2M3Ga9 (M = Rh, Ir)

The intermediate valence compounds Yb2M3Ga9 (M = Rh, Ir) exhibit an anisotropic magnetic susceptibility. We report measurements of the temperature dependence of the 4f occupation number, nf(T), for Yb2M3Ga9 as well as the magnetic inelastic neutron scattering spectrum Smag at 12 and 300 K for Yb2Rh3Ga9. Both nf(T) and Smag were calculated for the Anderson impurity model with crystal field terms within an approach based on the non-crossing approximation. These results corroborate the importance of crystal field effects in these materials; they also suggest that Anderson lattice effects are important to the physics of Yb2M3Ga9.

cond-mat.str-el

Antiferromagnetism in Pr3In: Singlet/triplet physics with frustration

We present neutron diffraction, magnetic susceptibility and specific heat data for a single-crystal sample of the cubic (Cu3Au structure) compound Pr3In. This compound is believed to have a singlet (Gamma1) groundstate and a low-lying triplet (Gamma4) excited state. In addition, nearest-neighbor antiferromagnetic interactions are frustrated in this structure. Antiferromagnetic order occurs below T_N = 12K with propagation vector (0, 0, 0.5 +/-δ) where δ\approx 1/12. The neutron diffraction results can be approximated with the following model: ferromagnetic sheets from each of the three Pr sites alternate in sign along the propagation direction with a twelve-unit-cell square-wave modulation. The three moments of the unit cell of 1 μ_B magnitude are aligned so as to sum to zero as expected for nearest-neighbor antiferromagnetic interactions on a triangle. The magnetic susceptibility indicates that in addition to the antiferromagnetic transition at 12K, there is a transition near 70K below which there is a small (0.005 μ_B) ferromagnetic moment. There is considerable field and sample dependence to these transitions. The specific heat data show almost no anomaly at TN = 12K. This may be a consequence of the induced moment in the Gamma1 singlet, but may also be a sample-dependent effect.

cond-mat.str-el