Ken Littrell

Spin echo scattering angle measurement at a pulsed neutron source

Two experiments were performed to adapt spin echo scattering angle measurement (SESAME) to pulsed neutron sources. SESAME is an interferometric method that provides enhanced resolution of neutron scattering angles without the loss of neutron intensity that results when collimation is used to improve angular resolution. The method uses the neutron equivalent of optical wave plates to produce a phase difference between the two neutron spin components of a polarized neutron beam. Because the wave plate is inclined to the neutron beam, this phase difference depends sensitively on the trajectory of the neutron. In the absence of a sample, a second wave plate, which is parallel to the first, undoes the phase difference introduced by the first wave plate, producing a polarization identical to that of the incident neutron beam. When a scattering sample is placed between the two neutron wave plates, the cancellation of the phase difference between the neutron spin states is not perfect and the resulting neutron-beam polarization is a measure of the distribution of scattering angles. In the first experiment, thin (30 and 60u2005µm-thick) magnetized Permalloy films were used as neutron wave plates. In a second experiment, current-carrying solenoids with triangular cross sections were used as birefringent prisms for neutrons. The arrangement of these prisms was such that they mimicked the effect of the neutron wave plates in the first experiment. In both experiments, correlation lengths in the scattering sample of about 1000u2005A were probed using very simple and inexpensive equipment. These experiments brought to light a number of advantages and disadvantages of implementing SESAME at pulsed neutron sources and provided insights into the relative merits of SESAME and traditional small-angle neutron scattering.

Structure and property correlations in FeS

Structure and composition of iron chalcogenides have a delicate relationship with magnetism and superconductivity. In this report we investigate the iron sulfide layered tetragonal phase (t-FeS), and compare with three-dimensional hexagonal phase (h-FeS). X-ray diffraction reveals the absence of structural transitions for both t- and h-FeS below room temperature, and gives phase compositions of Fe0.93(1)S and Fe0.84(1)S, respectively, for the samples studied here. The a lattice parameter of bigger than 3.68 A is significant for causing bulk superconductivity in iron sulfide, which is controlled by composition and structural details such as iron stoichiometry and concentration of vacancy. While h-FeS with a = 3.4436(1) A has magnetic ordering well above room temperature, our t-FeS with a =3.6779(8)A shows filamentary superconductivity below Tc = 4 K with less than 15% superconducting volume fraction. Also for t-FeS, the magnetic susceptibility shows an anomaly at ~ 15 K, and neutron diffraction reveals a commensurate antiferromagnetic ordering below TN = 116 K, with wave vector km= (0.25,0.25,0) and 0.46(2)uB/Fe. Although two synthesis routes are used here to stabilize t vs h crystal structures (hydrothermal vs solid-state methods), both FeS compounds order on two length-scales of ~1000 nm sheets or blocks and ~ 20 nm smaller particles, shown by neutron scattering. First principles calculations reveal a high sensitivity to the structure for the electronic and magnetic properties in t-FeS, predicting marginal antiferromagnetic instability for our compound (sulfur height of zS ~0.252) with an ordering energy of ~11 meV/Fe, while h-FeS is magnetically stable.

In situ neutron scattering study of nanoscale phase evolution in PbTe-PbS thermoelectric material

Introducing nanostructural second phases has proved to be an effective approach to reduce the lattice thermal conductivity and thus enhances the figure of merit for many thermoelectric materials. Studies of the formation and evolution of these second phases are essential to understanding material temperature dependent behaviors, improving thermal stabilities, as well as designing new materials. In this study, powder samples of the PbTe-PbS thermoelectric material were examined using in situ neutron diffraction and small angle neutron scattering (SANS) techniques between room temperature and elevated temperature up to 663u2009K, to explore quantitative information on the structure, weight fraction, and size of the second phase. Neutron diffraction data showed that the as-milled powder was primarily a solid solution prior to heat treatment. During heating, a PbS second phase precipitated out of the PbTe matrix around 500u2009K, while re-dissolution started around 600u2009K. The second phase remained separated from the ...

First data acquired on the extended Q-range small-angle neutron scattering (EQ-SANS) diffractometer at the Spallation Neutron Source

Initial experimental results are reported from the extended Q-range small-angle neutron scattering (EQ-SANS) diffractometer at the Spallation Neutron Source at Oak Ridge National Laboratory (ORNL). A generation-8 polyamidoamine dendrimer was measured and the conformation parameters (radius of gyration, thickness of the soft shell etc.) extracted by model fitting to the scattering data. The results are compared with data collected at the general-purpose small-angle neutron scattering (GP-SANS) beamline at the High-Flux Isotopic Reactor at ORNL and show that EQ-SANS is ready for scientific studies for the small-angle neutron scattering community.

Vortex lattice structure in BaFe2(As0.67P0.33)(2) via small-angle neutron scattering

We have observed a magnetic vortex lattice (VL) in BaFe2(As_{0.67}P_{0.33})2 (BFAP) single crystals by small-angle neutron scattering (SANS). With the field along the c-axis, a nearly isotropic hexagonal VL was formed in the field range from 1 to 16 T, which is a record for this technique in the pnictides, and no symmetry changes in the VL were observed. The temperature-dependence of the VL signal was measured and confirms the presence of (non d-wave) nodes in the superconducting gap structure for measurements at 5 T and below. The nodal effects were suppressed at high fields. At low fields, a VL reorientation transition was observed between 1 T and 3 T, with the VL orientation changing by 45{deg}. Below 1 T, the VL structure was strongly affected by pinning and the diffraction pattern had a fourfold symmetry. We suggest that this (and possibly also the VL reorientation) is due to pinning to defects aligned with the crystal structure, rather than being intrinsic.

Self-assembly of a semi-fluorinated diblock copolymer in a selective solvent

The self-assembly of a highly incompatible siloxane containing semi-fluorinated diblock copolymer, polytrifluoro propyl methylsiloxane-b-polystyrene (SiF-PS), in toluene, a selective solvent for polystyrene, was studied using Small Angle Neutron Scattering. Incompatibility is often enhanced by inserting fluorinated segments into one of the blocks and as a result not only the interchain interactions are changed but also the rigidity of the blocks. Herein the incorporation of siloxane into the backbone of a semi-fluorinated block maintains its flexibility and allows separation of the effects of direct interactions due to fluorine atoms from those of rigidity. Measurements were carried out in dilute solutions below 1 wt%, at volume fractions ϕSiF ranging from 0.0 to 0.5. The high incompatibility of the SiF block drives aggregation at low volume fractions of the SiF block, where spherical core–Gaussian shell aggregates are detected at ϕSiF = 0.16. In the symmetric SiF-PS complex fluid, elongated micelles were observed. The micelles exhibited unique temperature stability in comparison with the aggregates formed by diblock-copolymers in the lower segregation regime. As the temperature increases the micelles dissociate into free chains to form unimolecular micelles.

Modeling the Electrical Response of Waspaloy due to the Nucleation, Growth, and Coarsening of γ′

Waspaloy is a polycrystalline nickel-base superalloy used in disc rotors for gas turbine engines. Waspaloy, like other superalloys, is strengthened through the formation of the γ’ precipitate phase. As this precipitate phase evolves with processing and thermal exposure, it is desirable to non-destructively monitor the precipitate microstructural evolution. Electrical resistivity was used as such a non-destructive monitoring technique for aging temperatures ranging from 600°C to 800°C and aging times ranging between 2min and 263.5h. In the nucleation regime, a Johnson-Mehl-Avrami type equation was fit to the electrical response. For the growth and coarsening regimes, a volume distribution of precipitates was fit to the measured electrical resistivity. These fitting techniques were facilitated by microstructural data obtained from SEM imaging, X-ray diffraction, and small angle neutron scattering (SANS) measurements. For both cases, the models showed an excellent fit to the measured electrical data, implying that electrical resistivity is a viable technique for non-destructively monitoring the precipitate phase in Waspaloy.

Origin of dielectric relaxor behavior in PVDF-based copolymer and terpolymer films

Relaxor ferroelectrics exhibit frequency-dispersion of their dielectric permittivity peak as a function of temperature, the origin of which has been widely debated. Microscopic understanding of such behavior for polymeric ferroelectrics has presented new challenges since unlike traditional ceramic ferroelectrics, dielectric relaxation in polymers is a consequence of short-range molecular dynamics that are difficult to measure directly. Here, through careful analysis of atomic-level H-atom dynamics as determined by Quasi-elastic Neutron Scattering (QENS), we show that short-range molecular dynamics within crystalline domains cannot explain the macroscopic frequency-dispersion of dielectric properties observed in prototypical polyvinylidene-fluoride (PVDF)-based relaxor ferroelectrics. Instead, from multiscale quantitative microstructural characterization, a clear correlation between the amount of crystalline-amorphous interfaces and dielectric relaxation is observed, which indicates that such interfaces pl...

Vortex lattice structure inBaFe2(As0.67P0.33)2via small-angle neutron scattering

We have observed a magnetic vortex lattice (VL) in BaFe2(As_{0.67}P_{0.33})2 (BFAP) single crystals by small-angle neutron scattering (SANS). With the field along the c-axis, a nearly isotropic hexagonal VL was formed in the field range from 1 to 16 T, which is a record for this technique in the pnictides, and no symmetry changes in the VL were observed. The temperature-dependence of the VL signal was measured and confirms the presence of (non d-wave) nodes in the superconducting gap structure for measurements at 5 T and below. The nodal effects were suppressed at high fields. At low fields, a VL reorientation transition was observed between 1 T and 3 T, with the VL orientation changing by 45{deg}. Below 1 T, the VL structure was strongly affected by pinning and the diffraction pattern had a fourfold symmetry. We suggest that this (and possibly also the VL reorientation) is due to pinning to defects aligned with the crystal structure, rather than being intrinsic.

Vortex lattice structure in BaFe2(As0.67P0.33)2 by the small-angle neutron scattering technique

We have observed a magnetic vortex lattice (VL) in BaFe2(As_{0.67}P_{0.33})2 (BFAP) single crystals by small-angle neutron scattering (SANS). With the field along the c-axis, a nearly isotropic hexagonal VL was formed in the field range from 1 to 16 T, which is a record for this technique in the pnictides, and no symmetry changes in the VL were observed. The temperature-dependence of the VL signal was measured and confirms the presence of (non d-wave) nodes in the superconducting gap structure for measurements at 5 T and below. The nodal effects were suppressed at high fields. At low fields, a VL reorientation transition was observed between 1 T and 3 T, with the VL orientation changing by 45{deg}. Below 1 T, the VL structure was strongly affected by pinning and the diffraction pattern had a fourfold symmetry. We suggest that this (and possibly also the VL reorientation) is due to pinning to defects aligned with the crystal structure, rather than being intrinsic.