J. C. Lashley

Los Alamos National Laboratory, Los Alamos, California, United States

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Publications (156)302.18 Total impact

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    ABSTRACT: The thermal conductivity of uranium dioxide has been studied for over half a century, as uranium dioxide is the fuel used in a majority of operating nuclear reactors and thermal conductivity controls the conversion of heat produced by fission events to electricity. Because uranium dioxide is a cubic compound and thermal conductivity is a second-rank tensor, it has always been assumed to be isotropic. We report thermal conductivity measurements on oriented uranium dioxide single crystals that show anisotropy from 4 K to above 300 K. Our results indicate that phonon-spin scattering is important for understanding the general thermal conductivity behaviour, and also explains the anisotropy by coupling to the applied temperature gradient and breaking cubic symmetry.
    Nature Communications 01/2014; 5:4551. · 10.02 Impact Factor
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    ABSTRACT: We probe the volume collapse transition (ΔV/Vo ∼ 15%) between the isostructural γ and α phases (T ∼ 100 K) of Ce0.9Th0.1 using the Hall effect, three-terminal capacitive dilatometry, and electrical resistivity measurements. Hall effect measurements confirm the itinerant ground state as the carrier concentration increases by a factor of 7 in the α phase, γ phase (nH = 5.28 × 10(26) m(-3)), and the α phase (nH = 3.76 × 10(27) m(-3)). We were able to detect a noise spectrum consisting of avalanches while slowly varying the temperature through the hysteretic region. We surmise that the avalanches originate from intergranular stresses at the interfaces between partially transformed high-volume and low-volume phases. The statistical distribution of avalanches obey power laws with energy exponent ϵ ≃ 1.5. Hall effect measurements, combined with universal critical exponents, point to short electron mean-free percolation pathways and carrier localization at phase interfaces. Carrier localization was predicted many years ago for elemental cerium by Johansson (1974 Phil. Mag. 30 469).
    Journal of Physics Condensed Matter 12/2013; 26(3):035701. · 2.22 Impact Factor
  • R K Schulze, D C Wallace, J C Lashley
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    ABSTRACT: Valence band photoemission measurements have been made on crystalline and supercooled liquid gallium, and across the liquid and solid phases of bismuth and indium. Measurements are angle integrated and made using photon excitations of 21.21 and 40.81 eV. In all cases the Bloch states are destroyed upon melting and the free electron gas is constrained by a charge-neutral liquid. The spectra of indium show little change upon solidification, indicating a common electronic structure for crystalline and liquid phases. In contrast, the energy distribution curves for supercooled gallium and bismuth show large changes in the electronic structure from solid to liquid phases, giving rise to the formation of pseudogaps in the density of states at the Fermi energy, EF. Observations of this kind enable us to distinguish normal or anomalous melting from photoemission measurements.
    Journal of Physics Condensed Matter 10/2013; 25(46):465107. · 2.22 Impact Factor
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    ABSTRACT: Polyisoprene, (-CH2C(CH3)CH=CH2-)n, consists of isoprene (2--methyl--1,3--butadiene) molecules that are linked end--to--end to form long chains. There are two different isomers, cis and trans, with respect to configuration about the C=C double bond. Cis--polyisoprene, the main component in natural rubber derived originally from the Pará rubber tree, is a non--crystalline elastomer at room temperature. In contrast, trans--polyisoprene, derived originally from the gutta percha tree, is a crystalline solid that is rigid and tough. More interestingly, the trans isomer exhibits shape--memory properties, whereas the cis isomer does not. As for shape--memory transformations in alloys, trans--polyisoprene exhibits clear Af and Mf temperatures, with values 338 K and 300 K, respectively. Here we report thermodynamic and structural measurements of the shape--memory effect in trans--polyisoprene. We discuss our results in terms of the mechanism of shape--memory.
    03/2013;
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    ABSTRACT: For decades UO2 has been the most widely studied actinide oxide because of its technological importance as fuel material for nuclear reactors. Therefore there is a large interest in understanding its thermal, transport and thermodynamic properties. We present recent experimental results for the thermal conductivity and thermal expansion of high quality UO2 single crystal, obtained for different crystallographic directions, and compare with results of molecular dynamics simulations. We will discuss the implications of this study.
    03/2013;
  • A.C. Lawson, J.C. Lashley
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    ABSTRACT: We present a new analysis of the heat capacity of δ-phase Pu-5 at.% Al with a fit using a single-ion Kondo term and a low-temperature Schottky anomaly in addition to the Debye and linear terms. The Kondo and Schottky terms together contribute 1.2 R to the entropy at 300 K. We show how the extra entropy could affect the alloy phase diagrams of δ-phase Pu.
    Philosophical Magazine 01/2013; 93(18). · 1.60 Impact Factor
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    ABSTRACT: Low-temperature specific heat and thermal expansion measurements are used to study the hydrogen-based ferroelectric lawsonite over the temperature range 1.8 K ≤ T ≤ 300 K. The second-order phase transition near 125 K is detected in the experiments, and the low-temperature phase is determined to be improper ferroelectric and co-elastic. In the ferroelectric phase T ≤ 125 K, the spontaneous polarization P(s) is proportional to (1) the volume strain e(s), and (2) the excess entropy ΔS(e). These proportionalities confirm the improper character of the ferroelectric phase transition. We develop a structural model that allows the off-centering of hydrogen positions to generate the spontaneous polarization. In the low-temperature limit we detect a Schottky anomaly (two-level system) with an energy gap of Δ ∼ 0.5 meV.
    Journal of Physics Condensed Matter 05/2012; 24(25):255901. · 2.22 Impact Factor
  • D. J. Safarik, A. Llobet, J. C. Lashley
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    ABSTRACT: We address the error resulting from application of the harmonic Debye-Waller factor to anharmonic vibrations. The mean-square atomic displacement 〈u2〉 determined from the harmonic analysis is compared to values obtained from an exact anharmonic analysis. In the case of strong anharmonicity, we find that the harmonic approximation introduces at most a ∼25% error. The temperature dependence determined from the harmonic analysis follows that found from the exact anharmonic analysis. Errors introduced by the harmonic approximation are comparable in magnitude to the usual systematic errors associated with diffraction experiments and Rietveld refinements.
    Physical review. B, Condensed matter 05/2012; 85(17). · 3.77 Impact Factor
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    ABSTRACT: Despite large experimental and theoretical efforts the structure of the superconducting gap and the origin of the pairing mechanism in iron-based superconductors in still unresolved. Measurements of the low temperature specific heat and its magnetic response inside the superconducting state give important information about the symmetry of the gap. Here, we present results of our studies of codoped Ba0.55K0.45Fe1.95Co0.05As2 with a Tc of 32.5 K. The high quality of the material is marked by a pronounced peak at Tc as well as by a low residual specific heat γ0 = 2.4 mJ/mol K^2. We will discuss the implications of the new specific heat results on the symmetry of the order parameter in this system.
    02/2012;
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    ABSTRACT: Quantized waves obeying Bose-Einstein statistics will contribute a T^3/2 term to the specific heat if the dispersion relation goes as q2. We measure the magnetic and electric field dependence of the specific heat on the ferroelectric material tri-glycine sulphate (TGS) over the temperature range 0.05 K < T < 350 K. We detect a T^3/2 term in the specific heat in the low-temperature limit, which is taken to be the dielectric analog to magnetic spin wave. Near the Curie temperature (TC = 320 K), the shape of the specific-heat anomaly is thermally broadened. However, the anomaly changes to the characteristic sharp lambda-shape expected for a continuous transition with the application of either a magnetic field or electric field, giving the expected entropy change at TC of Rln2. These results are explained on the basis that the frequencies of optical dipole oscillations are split by the magnetic field, and the resulting gas of excitations are paramagnetic. Consequently they contribute to the specific heat near TC, which increases with magnetic field.
    02/2012;
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    ABSTRACT: The gamma to alpha isostructural transition in the Ce(0.9-x)La(x)Th(0.10) system is measured as a function of La alloying and external pressure up to 1 Mbar using magnetic susceptibility. We probe a line of discontinuous transitions, as indicated by the change in volume, decreasing exponentially from 118 K to close to 0 K with increasing La doping, and the transition changes from being first order to continuous at a critical concentration close to x = 0.14. At the tricritical point, the magnetic susceptibility increase rapidly near the critical concentration and approaches large values at x= 0.35 signifying that a heavy Fermi-liquid state evolves at large doping near the critical concentration. The Wilson ratio reaches a value above two for a narrow range of concentrations where the specific heat and susceptibility vary most rapidly with the doping concentration.
    02/2012;
  • Douglas Safarik, Anna Llobet, Jason Lashley
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    ABSTRACT: The Debye-Waller factor relates the intensities of the Bragg peaks to the mean square displacements of the atoms. In the structural refinement of diffraction data it is standard practice to use the harmonic expression for Debye-Waller factor. For most materials and conditions the phonons are only mildly anharmonic, thus the harmonic assumption is a good one. For some materials and conditions, however, the phonons can be strongly anharmonic, and thus the harmonic assumption is physically unrealistic. As examples we cite the rattling atoms in clathrates and skutterudites, and atoms participating in displacive phase transitions. In the present study we investigate the error associated with using the harmonic Debye--Waller factor to analyze anharmonic vibrations. We find that even for strongly anharmonic potentials, such as a double well, the mean square displacements deduced using the harmonic approximation are at most 15% larger than those deduced using a full anharmonic analysis. Furthermore, the quasi-harmonic and anharmonic values have nearly the same temperature dependences. We conclude that the error introduced by using the harmonic approximation is comparable to or smaller than the usual errors associated with measurement and refinement of diffraction patterns.
    02/2012;
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    ABSTRACT: We have used a suite of diffraction, thermodynamic, and transport measurements to study the localized rattling of Al guest atoms in VAl10.1. The mean-square displacement of the rattling atom shows a concave-down temperature dependence. This is characteristic of an anharmonic vibration, the frequency of which increases with amplitude, akin to a particle in a box. We find that the rattling is best described in terms of a sixth-order interatomic potential, with negligible contributions from harmonic and quartic terms. The rattler has a characteristic temperature of θRM=21 K and couples strongly to both the acoustic phonons and conduction electrons. The coupling to the phonons is evident from the large value of the Grüneisen parameter, which increases with decreasing temperature to Γ≈43 at 5 K. Below 6 K, the electrical resistivity varies as T3, which can be explained in terms of electron scattering from damped sixth-order vibrations. VAl10.1 is a superconductor below Tc=1.53 K, with an upper critical field of ∼1 kG.
    Physical review. B, Condensed matter 01/2012; 85(1). · 3.77 Impact Factor
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    ABSTRACT: We have measured the dose dependence of the degree of amorphization of titanite, CaTiSiO(5). Titanite is an often metamict mineral which has been considered as a matrix for the encapsulation of radiogenic waste, such as Pu. The amorphous fraction p of geologically irradiated samples (ages between 0.3 and 1 Ga) follows p = 1 - exp(-B(a)D) where D is the total dose and the characteristic amorphization mass is B(a) = 2.7(3) × 10(-19) g. Amorphization follows the direct impact mechanism where each α-decay leads to a recoil of the radiogenic atoms (mostly Th and U), which then, in turn, displaces some 5000 atoms of the titanite matrix. The amorphization behaviour is almost identical with that of zircon, ZrSiO(4), which has a similar molecular mass. While the recrystallization mechanism and elastic behaviour of the two minerals are very different, we do not find significant differences for the amorphization mechanism. Our samples have undergone little reheating over their geological history, since heating over 800 K would lead to rapid recrystallization for which we have found no evidence.
    Journal of Physics Condensed Matter 12/2011; 24(5):052202. · 2.22 Impact Factor
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    ABSTRACT: We report an experimental determination of the dispersion of the soft phonon mode along [100] in uranium as a function of pressure. The energies of these phonons increase rapidly, with conventional behavior found by 20 GPa, as predicted by recent theory. New calculations demonstrate the strong pressure (and momentum) dependence of the electron-phonon coupling, whereas the Fermi-surface nesting is surprisingly independent of pressure. This allows a full understanding of the complex phase diagram of uranium and the interplay between the charge-density wave and superconductivity.
    Physical Review Letters 09/2011; 107(13):136401. · 7.73 Impact Factor
  • A C Lawson, J C Lashley
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    ABSTRACT: In this paper we apply the Aptekar-Ponyatovsky (AP) regular solution thermodynamic model to the analysis of experimental data for the coefficient of thermal expansion (CTE) and determine the AP model parameters for unalloyed cerium metal, Ce-Th-La alloys, and Pu-Ga alloys. We find that the high temperature CTE of cerium metal follows the predictions of the AP model based on low temperature, high pressure data. For Ce-Th-La alloys we use the AP parameters to track the suppression of the first-order γ-α cerium transition. We show the AP model accounts for the negative CTE observed for Pu-Ga alloys and is equivalent to an earlier invar model. Finally, we apply the AP parameters obtained for Pu-Ga alloys to rationalize the observed δ-α transformation pressures of these alloys. We show that the anomalous values of the Grüneisen and Grüneisen-Anderson parameters are important features of the thermal properties of plutonium. A strong analogy between the properties of plutonium and cerium is confirmed.
    Journal of Physics Condensed Matter 09/2011; 23(36):365803. · 2.22 Impact Factor
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    ABSTRACT: We study some dynamic aspects of a Mott transition in a rare-earth alloy Ce0.90Th0.10 by resonant-ultrasound spectroscopy (RUS), electrical-transport, and thermal-expansion measurements. In the temperature range spanning the first-order transition, we observe a stiffening of the elastic response that is associated with a continuous front propagation (e.g. solitons). A defining characteristic of a mixed phase regime, slow scanning rates (0.01 K/min) show these solitons to be superimposed with jerks and avalanches in all three data sets: RUS, resistivity, and thermal expansion data. Analysis of the avalanche data give power law distributions with critical exponents P(E)=E^n for energy, in the case of thermal expansion data and length, in the case of electrical transport data.
    03/2011;
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    ABSTRACT: Iron is a ubiquitous impurity in metamict (radiation-damaged and partially amorphized) materials such as titanite (CaSiTiO(5)). Using (57)Fe Mössbauer spectroscopy we find that iron in metamict titanite is partitioned between amorphous and crystalline regions based on valence. Trivalent iron exists in the crystalline titanite matrix whereas divalent iron exists almost exclusively in radiation-amorphized regions. We find that the relative abundances of the oxidation states correlate with the volume fraction of amorphous and crystalline regions. Our data also show that oxidation of iron proceeds along with the recrystallization of the amorphized regions. Recrystallization is confirmed to occur over the range 700 °C < T < 925 °C, and no further structural changes are observed at higher temperatures. It is surprising that our Mössbauer measurements show divalent iron to be surrounded by titanite with a high degree of short-range structural order in the amorphized regions. This observation is fundamentally different from other metamict materials such as zircon (ZrSiO(4)), where amorphized regions show no short-range order.
    Journal of Physics Condensed Matter 03/2011; 23(10):105402. · 2.22 Impact Factor
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    ABSTRACT: In this article we examine the low-temperature specific heat of slow-cooled Cu(0.2)Ag(2.8)SbSeTe(2) and the thermoelectric performance of quenched samples. We find that the low-temperature specific heat is dominated by two Einstein terms of approximate energies of 2.5 and 5 meV. The specific-heat behavior is consistent with the amorphous low-temperature thermal conductivity behavior and validates the glassy nature of the structure. We performed the synthesis of quenched samples in an attempt to eliminate the presence of micro-cracks, whose existence presumably enhances electronic scattering. We find that quenching eliminates the presence of micro-cracks but does not result in an improvement of the figure of merit. Specifically, the highest ZT obtained in the quenched samples (ZT = 1.5), though very competitive, is still significantly less that the ZT obtained in the slow-cooled samples (ZT = 1.75).
    Journal of Physics Condensed Matter 03/2011; 23(13):135305. · 2.22 Impact Factor

Publication Stats

1k Citations
302.18 Total Impact Points

Institutions

  • 2000–2013
    • Los Alamos National Laboratory
      • • Materials Science and Technology Division
      • • Metallurgy Group
      Los Alamos, California, United States
  • 2010–2012
    • University of Cambridge
      • • Department of Earth Sciences
      • • Department of Physics: Cavendish Laboratory
      Cambridge, ENG, United Kingdom
  • 2011
    • University of British Columbia - Vancouver
      • Department of Earth and Ocean Sciences
      Vancouver, British Columbia, Canada
  • 2008
    • Институт физики высоких энергий
      Protvino, Moskovskaya, Russia
  • 2004–2007
    • National High Magnetic Field Laboratory
      Tallahassee, Florida, United States
  • 2005
    • Shizuoka University
      • Department of Physics
      Shizuoka-shi, Shizuoka-ken, Japan
  • 2001
    • Lawrence Berkeley National Laboratory
      • Geochemistry Department
      Berkeley, California, United States
    • Brigham Young University - Idaho
      Los Alamos, New Mexico, United States