arXiv subjects

C. H. Booth

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

34 records · Page 2Linked to original sources

arXiv2004

Direct Observation of High-Temperature Polaronic Behavior In Colossal Magnetoresistive Manganites

The temperature dependence of the electronic and atomic structure of the colossal magnetoresistive oxides $La_{1-x}Sr_{x}MnO_{3}$ (x = 0.3, 0.4) has been studied using core and valence level photoemission, x-ray absorption and emission, and extended x-ray absorption fine structure spectroscopy. A dramatic and reversible change of the electronic structure is observed on crossing the Curie temperature, including charge localization and spin moment increase of Mn, together with Jahn-Teller distortions, both signatures of polaron formation. Our data are also consistent with a phase-separation scenario.

cond-mat.str-el↗

arXiv2003

Structural properties of the geometrically frustrated pyrochlore Tb2Ti2O7

Although materials that exhibit nearest-neighbor-only antiferromagnetic interactions and geometrical frustration theoretically should not magnetically order in the absence of disorder, few such systems have been observed experimentally. One such system appears to be the pyrochlore Tb2Ti2O7. However, previous structural studies indicated that Tb2Ti2O7 is an imperfect pyrochlore. To clarify the situation, we performed neutron powder diffraction (NPD) and x-ray absorption fine structure (XAFS) measurements on samples that were prepared identically to those that show no magnetic order. The NPD measurements show that the long-range structure of Tb2Ti2O7 is well ordered with no structural transitions between 4.5 and 600 K. In articular, mean-squared displacements (u^2's) for each site follow a Debye model with no offsets. No evidence for Tb/Ti site interchange was observed within an upper limit of 2%. Likewise, no excess or deficiency in the oxygen stoichiometry was observed, within an upper limit of 2% of the nominal pyrochlore value. Tb L3- and Ti K-edge XAFS measurements from 20-300 K similarly indicate a well-ordered local structure. Other aspects of the structure are considered. We conclude that Tb2Ti2O7 has, within experimental error, an ideal, disorder-free pyrochlore lattice, thereby allowing the system to remain in a dynamic, frustrated spin state to the lowest observed temperatures.

cond-mat.str-el↗

arXiv2003

Improved self-absorption correction for fluorescence measurements of extended x-ray absorption fine-structure

Extended x-ray absorption fine-structure (EXAFS) data collected in the fluorescence mode are susceptible to an apparent amplitude reduction due to the self-absorption of the fluorescing photon by the sample before it reaches a detector. Previous treatments have made the simplifying assumption that the effect of the EXAFS on the correction term is negligible, and that the samples are in the thick limit. We present a nearly exact treatment that can be applied for any sample thickness or concentration, and retains the EXAFS oscillations in the correction term.

cond-mat↗

arXiv2002

Changes in non-Fermi liquid behavior with annealing due to lattice disorder in UCu_4Pd

The magnetic and electronic properties of non-Fermi liquid UCu_4Pd depend on annealing conditions. Local structural changes due to this annealing are reported from U L_III- and Pd K-edge x-ray absorption fine-structure measurements. In particular, annealing decreases the fraction of Pd atoms on nominally Cu 16e sites and the U-Cu pair-distance distribution width. This study provides quantitative information on the amount of disorder in UCu_4Pd and allows an assessment of its possible importance to the observed non-Fermi liquid behavior.

cond-mat.str-el↗

arXiv2002

Effects of lattice disorder in the UCu_(5-x)Pd_(x) system

The UCu(5-x)Pd(x) system exhibits non-Fermi liquid (NFL) in the thermodynamic and transport properties at low temperatures for Pd concentrations 0.9 <~ x <~ 1.5. The local structure around the U, Cu, and Pd atoms has been measured for 0 <= x <= 1.5 using the X-ray Absorption Fine Structure (XAFS) technique in order to quantify the effects of lattice disorder on the NFL properties. A model which allows a percentage of the Pd atoms to occupy nominal Cu (16e) sites, s, was used to fit the Pd and Cu K edge and U L(III) edge data. Pd/Cu site interchange was found to occur in all samples (x != 0), reaching a minimum value of s ~0.17 at x = 0.7 and increasing monotonically to s ~ 0.4 at x=1.5. These data also determine the static disorder the nearest neighbor U--Cu pairs. The results indicate that the measured U--Cu static disorder is not sufficient to explain the NFL behavior of the magnetic susceptibility within the single-ion Kondo disorder model and casts doubt on the applicability of this model to UCu(5-x)Pd(x).

cond-mat.str-el↗

arXiv2002

Studies of Vibrational Properties in Ga Stabilized d-Pu by Extended X-ray Absorption Fine Structure

Temperature dependent extended x-ray absorption fine structure (EXAFS) spectra were measured for a 3.3 at% Ga stabilized Pu alloy over the range T= 20 - 300 K at both the Ga K-edge and the Pu L_III-edge. The temperature dependence of the pair-distance distribution widths, σ(T) was accurately modeled using a correlated-Debye model for the lattice vibrational properties, suggesting Debye-like behavior in this material. We obtain pair- specific correlated-Debye temperatures, Θ_cD, of 110.7 +/- 1.7 K and 202.6 +/- 3.7 K, for the Pu-Pu and Ga-Pu pairs, respectively. These results represent the first unambiguous determination of Ga-specific vibrational properties in PuGa alloys, and indicate the Ga-Pu bonds are significantly stronger than the Pu-Pu bonds. This effect has important implications for lattice stabilization mechanisms in these alloys.

cond-mat.str-el↗

arXiv2001

Two energy scales and slow crossover in YbAl3

Experimental results for the susceptibility, specific heat, 4f occupation number, Hall effect and magnetoresistance for single crystals of YbAl$_{3}$ show that, in addition to the Kondo energy scale $k_{B}T_{K}$ $% \sim $ 670K, there is a low temperature scale $T_{coh}<50$K for the onset of coherence. Furthermore the crossover from the low temperature Fermi liquid regime to the high temperature local moment regime is slower than predicted by the Anderson impurity model. These effects may reflect the behavior of the Anderson Lattice in the limit of low conduction electron density.

cond-mat.str-el↗

arXiv2001

Slow crossover in YbXCu4 intermediate valence compounds

We compare the results of measurements of the magnetic susceptibility Chi(T), the linear coefficient of specific heat Gamma(T)=C(T)/T and 4f occupation number nf(T) for the intermediate valence compounds YbXCu4 (X = Ag, Cd, In, Mg, Tl, Zn) to the predictions of the Anderson impurity model, calculated in the non-crossing approximation (NCA). The crossover from the low temperature Fermi liquid state to the high temperature local moment state is substantially slower in the compounds than predicted by the NCA; this corresponds to the ''protracted screening'' recently predicted for the Anderson Lattice. We present results for the dynamic susceptibility, measured through neutron scattering experiments, to show that the deviations between theory and experiment are not due to crystal field effects, and we present x-ray-absorption fine-structure (XAFS) results that show the local crystal structure around the X atoms is well ordered, so that the deviations probably do not arise from Kondo Disorder. The deviations may correlate with the background conduction electron density, as predicted for protracted screening.

cond-mat.str-el↗

arXiv2000

Temperature dependent changes of the Mn 3d and 4p bands near T$_c$ in Colossal Magnetoresistance systems: a XANES study of La$_{1-x}$Ca$_x$MnO$_3$

We report high-resolution X-ray Absorption Near Edge Structure (XANES) measurements at the Mn K-edge as a function of temperature, for La$_{1-x}$Ca$_x$MnO$_3$ samples, with a focus mainly on the pre-edge region. Small peaks labeled A$_1$-A$_3$ are observed which corresponds to 1s-3d dipole-transitions, made weakly allowed via a hybridization of Mn 4p states with Mn 3d states on {\it neighboring} atoms. Adjusting the parameters in an LSDA calculation to approximately match the experimental A$_1$-A$_2$ splitting yields U = 4 eV and J$_H$ = 0.7 eV. For colossal magnetoresistance samples, A$_1$ decreases with T while A$_2$ increases with T below T$_c$, which shows that the 3d bands change significant as T moves through T$_c$. There are also small changes in the shape of the main edge (1s-4p transitions).

cond-mat↗

arXiv2000

Local lattice disorder in the geometrically-frustrated spin glass pyrochlore Y2Mo2O7

The geometrically-frustrated spin glass Y2Mo2O7 has been considered widely to be crystallographically ordered with a unique nearest neighbor magnetic exchange interaction, J. To test this assertion, we present x-ray-absorption fine-structure results for the Mo and Y K edges as a function of temperature and compare them to results from a well-ordered pyrochlore, Tl2Mn2O7. We find that the Mo-Mo pair distances are significantly disordered at approximately right angles to the Y-Mo pairs. These results strongly suggest that lattice disorder nucleates the spin-glass phase in this material.

cond-mat.stat-mech↗

arXiv1998

Pd/Cu Site Interchange and Non-Fermi-Liquid Behavior in UCu_4Pd

X-ray-absorption fine-structure measurements of the local structure in UCu_4Pd are described which indicate a probable lattice-disorder origin for non-Fermi-liquid behavior in this material. Short Pd-Cu distances are observed, consistent with 24 +/- 3% of the Pd atoms occupying nominally Cu sites. A "Kondo disorder" model, based on the effect on the local Kondo temperature T_K of this interchange and some additional bond-length disorder, agrees quantitatively with previous experimental susceptibility data, and therefore also with specific heat and magnetic resonance experiments.

cond-mat.str-el↗

arXiv1996

Evidence of magnetization-dependent polaron formation in La$_{1-x}A_x$MnO$_3$, $A$=Ca, Pb

X-ray-absorption fine-structure measurements at the Mn $K$-edge as a function of temperature were performed on samples of La$_{1-x}$Ca$_x$MnO$_3$ and La$_{0.67}$Pb$_{0.33}$MnO$_3$. All samples have a metal-insulator (MI) transition near the ferromagnetic transition, except the Ca$_{0.5}$ sample, which does not have a MI transition. Near $T_c$ for the MI samples, the Debye-Waller $σ^2$ for the Mn-O atom-pair increases rapidly with temperature. This non-thermal disorder is mostly along the direction of the neighboring oxygens. These results strongly suggest small polarons which are delocalized by a finite magnetization.

cond-mat↗

arXiv1996

Local structure study about Co in YBa$_2$(Cu$_{1-x}$Co$_x$)$_3$O$_{7-δ}$ thin films using polarized XAFS

We have studied the local structure around Co in YBa$_2$(Cu$_{1-x}$Co$_x$)$_3$O$_{7-δ}$ thin films with three different concentrations: x=0.07, 0.10, 0.17, and in a PrBa$_2$(Cu$_{1-x}$Co$_x$)$_3$O$_{7-δ}$ thin film of concentration x=0.05 using the X-ray Absorption Fine Structure (XAFS) technique. Data were collected at the Co $K$-edge with polarizations both parallel and perpendicular to the film surface. We find that the oxygen neighbors are well ordered and shortened in comparison with YBCO Cu-O values to 1.80 Å and 1.87 Å in the $c$-axis and $ab$-plane, respectively. A comparison of further neighbors in the thin film and powder data show that these peaks in the film are suppressed in amplitude relative to the powder samples, which suggests there is more disorder and/or distortions of the Co environment present in the thin films.

cond-mat↗

arXiv1996

Comparison of local structure measurements from c-axis polarized XAFS between a film and a single crystal of YBCO as a function of temperature

We have performed fluorescence x-ray absorption fine-structure (XAFS) measurements from 20-200 K on a 5000 Å, c-axis film of YBa_2Cu_3O_{7-δ} (YBCO) on MgO (Tc=89 K) using photons polarized perpendicular to the film. These data are compared to YBCO data from a single crystal and from a film on LaAlO_3 with the same Tc. The main difference between the single crystal and the film data is that while the single crystal data is well described by a two-site axial oxygen [O(4)] distribution, we see no evidence for such a distribution in either thin film sample. We place an upper limit on the size ofan axial oxygen splitting for the film on MgO at < 0.09 Å. Therefore, the magnitude of the splitting is not directly related to Tc. Fits to the temperature dependent data from the YBCO film on MgO indicate that all bonds show a smooth change of their broadening factor σ, except the Cu-O(4) bonds, which show an increase in σin the vicinity of Tc, followed by a decrease of the same magnitude. Such a feature does not occur in diffraction measurements. Since XAFS measurements of σinclude any correlation between the atoms in a given bond, we conclude that the O(4) position becomes less correlated with the Cu positions near Tc. Correlation measurements of these and several further near-neighbors are also reported.

cond-mat↗

arXiv1994

Local Disorder in the Oxygen Environment Around Praseodymium in YBCO:Pr from X-ray Absorption Fine Structure

We present K-edge XAFS (X-Ray Absorption Fine Structure) data for various concentrations of Pr in Y$_{1- x}$Pr$_{x}$Ba$_{2}$Cu$_{3}$O$_{7}$. The character of the Pr K-edge XAFS data indicate that most of the Pr substitutes onto the Y site and is well ordered with respect to the unit cell. These data also show that the amplitude of the first Pr-O peak is greatly reduced when compared to the first Y-O peak in pure YBCO, and decreases with increasing Pr concentration. In contrast, the Y K-edge data for these alloys show little if any change in the oxygen environment, while the Cu K-edge data show a 10\% reduction in the first Cu-O peak. Fits to the Pr data suggest that some oxygen atoms about the Pr become disordered and/or distorted; most of the Pr-O nearest- neighbor distances are 2.45 Å, but about 15-40\% of them are in a possibly broadened peak at 2.27$^{+0.03}_{-0.12}$ Å. The Cu K-edge XAFS data show a slight broadening but no loss of oxygens, which is consistent with a radial distortion of the Pr-O bond. The existence and the size of these two bond lengths is consistent with a mixture of Pr$^{3+}$ and Pr$^{4+}$ bonds, and to a formal valence of +3.33$^{+0.07}_{-0.18}$ for the Pr ion. This paper should be published in Feb. 1994 in Phys. Rev. B.

cond-mat↗

arXiv1994

X-ray Absorption Fine Structure in Embedded Atoms

Oscillatory structure is found in the atomic background absorption in x-ray-absorption fine structure (XAFS). This atomic-XAFS or AXAFS arises from scattering within an embedded atom, and is analogous to the Ramsauer-Townsend effect. Calculations and measurements confirm the existence of AXAFS and show that it can dominate contributions such as multi-electron excitations. The structure is sensitive to chemical effects and thus provides a new probe of bonding and exchange effects on the scattering potential.

cond-mat↗