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At least 613 records · Page 34

Thermal neutron imaging detector with wavelength shifting fiber and digital readout

Here, we developed a large area, digital thermal neutron imaging detector. The detector uses a 6 LiF/ZnS(Ag) neutron-sensitive scintillator combined with wavelength shifting fiber technology. The signals from fiber channels are amplified, integrated, and digitized using individual analog-to-digital converters for each channel. The neutron position is determined from the digitized signal using a least-squares gaussian-fitting algorithm. The detector size was 77 × 38 cm 2 (2926 cm 2 ), it provided 1.3 mm resolution, and its resolution can further be improved. The detector was designed for a powder diffraction neutron scattering beamline and provided substantial improvement of d-space resolution compared with existing detectors. This detector may have broader applications due to its large area and high spatial resolution extended over its large area.

6LiF/ZnS(Ag) scintillator↗

Unprecedented non-hysteretic superelasticity of [001]-oriented NiCoFeGa single crystals

Superelasticity associated with the martensitic transformation has found a broad range of engineering applications. However, the intrinsic hysteresis and temperature sensitivity of the first-order phase transformation significantly hinder the usage of smart metallic components in many critical areas. In this paper, we report a large superelasticity up to 15.2% strain in [001]-oriented NiCoFeGa single crystals, exhibiting non-hysteretic mechanical responses, a small temperature dependence and high-energy-storage capability and cyclic stability over a wide temperature and composition range. In situ synchrotron X-ray diffraction measurements show that the superelasticity is correlated with a stress-induced continuous variation of lattice parameter accompanied by structural fluctuation. Neutron diffraction and electron microscopy observations reveal an unprecedented microstructure consisting of atomic-level entanglement of ordered and disordered crystal structures, which can be manipulated to tune the superelasticity. The discovery of the large elasticity related to the entangled structure paves the way for exploiting elastic strain engineering and development of related functional materials. NiCoFeGa single crystals exhibit large non-hysteretic superelasticity over broad temperature and composition ranges. It is attributed to the continuous phase transition with applied stress, which is related to the fluctuation of entangled ordered and disordered crystal structures.

36 MATERIALS SCIENCE↗

Demonstration of neutron time-of-flight diffraction with an event-mode imaging detector

Neutron diffraction beamlines have traditionally relied on deploying large detector arrays of 3 He tubes or neutron-sensitive scintillators coupled with photomultipliers to efficiently probe crystallographic and microstructure information of a given material. Given the large upfront cost of custom-made data acquisition systems and the recent scarcity of 3 He, new diffraction beamlines or upgrades to existing ones demand innovative approaches. This paper introduces a novel Timepix3-based event-mode imaging neutron diffraction detector system as well as first results of a silicon powder diffraction measurement made at the HIPPO neutron powder diffractometer at the Los Alamos Neutron Science Center. Notably, these initial measurements were conducted simultaneously with the 3 He array on HIPPO, enabling direct comparison. Data reduction for this type of data was implemented in the MAUD code, enabling Rietveld analysis. Results from the Timepix3-based setup and HIPPO were benchmarked against McStas simulations, showing good agreement for peak resolution. With further development, systems such as the one presented here may substantially reduce the cost of detector systems for new neutron instrumentation as well as for upgrades of existing beamlines.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Status Report on Development of a Cask to Enable Pulsed Neutron Characterization of Irradiated Fuel

We present the design of a shielding cask that allows pulsed neutron characterization of irradiated fuel rodlets prior to their destructive examination in hot cells. The goal is to provide complementary and informative measurements that will inform subsequent hot cell PIE examinations by identifying typical and atypical regions with respect to microstructure, tomographic data, or isotope densities. Time-of-flight neutron diffraction has the potential to offer efficient, non-destructive and non-contact microstructural characterization of irradiated fuel pins with spatial resolution of 1 mm3 to 1 cm3 while for energy-resolved neutron imaging (and by extension tomography) a resolution of 100 μm was demonstrated. The potential results include crystallinity vs. amorphous volumes and microstructural information such as phase compositions and textures from the diffraction data as well as distances (e.g. pellet to cladding), cracks, and isotopic distributions of minor actinides, fission products as well as fission gas partial pressures e.g. in the plenum from energy resolved neutron imaging. The capability will identify regions of atypical behavior and provide cost effective bulk characterization of entire samples prior to destructive evaluation in hot cells. This effort is a collaboration between LANL, INL, ORNL, and UC Berkeley. A key facet of the initiative is the ability to cost effectively ship irradiated fuels from INL to the pulsed spallation neutron source at LANSCE. The irradiated fuel would be loaded in the custom designed cask (designated RaMHaM) at INL hot cells which then could be shipped in a BRR Type B shipment container between INL and LANL. No hot cell is required after the loading of the sample at INL in the pathway laid out in this report, greatly simplifying handling at LANL.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Structure and properties of densified silica glass: characterizing the order within disorder

The broken symmetry in the atomic-scale ordering of glassy versus crystalline solids leads to a daunting challenge to provide suitable metrics for describing the order within disorder, especially on length scales beyond the nearest neighbor that are characterized by rich structural complexity. Here, we address this challenge for silica, a canonical network-forming glass, by using hot versus cold compression to (i) systematically increase the structural ordering after densification and (ii) prepare two glasses with the same high-density but contrasting structures. The structure was measured by high-energy X-ray and neutron diffraction, and atomistic models were generated that reproduce the experimental results. The vibrational and thermodynamic properties of the glasses were probed by using inelastic neutron scattering and calorimetry, respectively. Traditional measures of amorphous structures show relatively subtle changes upon compacting the glass. The method of persistent homology identifies, however, distinct features in the network topology that change as the initially open structure of the glass is collapsed. The results for the same high-density glasses show that the nature of structural disorder does impact the heat capacity and boson peak in the low-frequency dynamical spectra. Densification is discussed in terms of the loss of locally favored tetrahedral structures comprising oxygen-decorated SiSi 4<:sub> tetrahedra.

36 MATERIALS SCIENCE↗

Deviation from the dipole-ice model in the spinel spin-ice candidate MgEr 2 Se 4

In spin-ice research, small variations in structure or interactions drive a multitude of different behaviors, yet the collection of known materials relies heavily on the “227” pyrochlore structure. Here, we present thermodynamic, structural, and inelastic-neutron-scattering data on a spin-ice material, MgEr 2 Se 4 , which contributes to the relatively underexplored family of rare-earth spinel chalcogenides. X-ray and neutron diffraction confirm a normal spinel structure and place Er 3+ moments on an ideal pyrochlore sublattice. Measurement of crystal electric field excitations with inelastic neutron scattering confirms that the moments have perfect Ising character, and further identifies the ground-state Kramers doublet as having dipolar-octupolar form with a significant multipolar character. Heat capacity and magnetic neutron diffuse scattering have icelike features, but are inconsistent with Monte Carlo simulations of the nearest-neighbor and next-nearest-neighbor dipolar spin-ice (DSI) models. A significant remnant entropy is observed as T → 0 K, but again falls short of the full Pauling expectation for DSI, unless significant disorder is added. We show that these observations are fully in line with what has been recently reported for CdEr 2 Se 4 , and point to the importance of quantum fluctuations in these materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Influence of Abrasive Grinding on Through-Section Residual Stresses on Bearing Steel

In today’s industrial world, bearings are used in traditional applications such as automotive, steel mills, paper mills, railways as well as high precision applications such as aerospace, medical, renewable energy etc. Regardless of application, residual stresses play an important role in the service life of a bearing. In general, bearings experience Hertzian stresses in the order of 2-3 GPa with maximum stresses generated in the subsurface. Depending upon the magnitude and nature (tensile or compressive), the residual stresses enhance or reduce the application stresses. The residual stresses are generated during each stage of manufacturing process. For bearing components, the manufacturing stages include – tube rolling, green machining followed by heat treatment and final finishing. Majority of bearings are finished using abrasive grinding to achieve the final size and shape. The work holding and material removal during the grinding process can cause significant distortion. Distortion of bearing components is ab significant issue, especially for thin sectioned components, leading to high scrap rates. In this study, diffraction was utilized to understand the evolution of through thickness residual stresses after abrasive grinding on a thin walled bearing component. The results from neutron diffraction were coupled with distortion measurement especially the out of roundness to understand the effect of the final processing on the residual stress state present in the bearings.

Bedekar, Vikram↗

RICH (Robotic Interface Control & Handling) System for VULCAN

High flux neutron beam and high efficiency detectors warrant quick turn arounds of neutron diffraction measurements at the engineering materials diffractometer VULCAN. Efficient change and alignment of samples and automatic measurements at VULCAN are desired for better use of neutron beam time by users. In this work, we aim to develop a proof-of-concept Robotic Interactive Control & Handling System (RICH) for sample handling at VULCAN that could assist high throughput experiments and reduce the overhead time significantly. This was realized by a six-axis desktop robot with trained AI models. The trained AI models can recognize and locate samples in various types of positions in a live video stream. In addition, we developed smart algorithms which used our models on multiple cameras to recognize where samples are with respect to multiple point of views, and then using user-inputted parameters, align them to perform complex measurements.

42 ENGINEERING↗

Complex Structural Disorder in a Polar Orthorhombic Perovskite Observed through the Maximum Entropy Method/Rietveld Technique

Ambient pressure stable perovskite oxides with all Bi3+ on the A-site are rare, with only four examples known. Due to the lone pair on Bi 3+ , these materials are seen as the best alternative to Pb-based piezoelectrics, which are used widely in society. The industry standard piezoelectric, Pb (Zr 1 – x Ti x )O 3 , relies on the [001] polarization of PbTiO 3 , but there are currently no ambient pressure stable Bi-based perovskites with this polarization vector, preventing the creation of an analogous system. We present the full structural analysis of the orthorhombic phase of (1 – x)Bi (Ti 3/8 Fe 2/8 Mg 3/8 )O 3 – x CaTiO 3 , which crystallizes in Pna2 1 symmetry with [001] polarization. This symmetry is rare and has only been reported twice for perovskites at ambient conditions. Analysis of maximum entropy method (MEM) models using synchrotron radiation powder X-ray diffraction reveals a disordered A-site configuration, and the MEM/Rietveld technique generates a structural model of this extreme disorder. Combined Rietveld analysis of X-ray and neutron diffraction data yields an accurate description of the local A-site configuration, which we use to understand our dielectric, ferroelectric, and piezoelectric measurements. These results give insight into how to stabilize this unique symmetry and inspire new design principles for Bi-based piezoelectrics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Complete Status Report Documenting the Development of Friction Stir Welding for Producing a Butt Joint in Thin Wall Tubing of ODS Alloys

A challenging attempt using friction stir welding to produce a butt joint between two 1.0 mm thick plates of 14YWT was nearly successful. The modified tool pin mostly penetrated the thickness of the adjoined thin plate samples resulting in a small blunt notch on the bottom surface of the butt joint. A bend occurred in the thin plate sample due to formation of stresses from clamping the thin plate sample during FSW. The peak displacement of the bend occurred along the center line of the butt joint. The weld zone showed good microstructure mixing with some flashing mostly on the retreating side that suggested excess heat input by friction between the traveling and spinning tool pin and thin plates of 14YWT. Neutron diffraction experiments were performed on the bent sample of 14YWT to measure the residual stresses in the butt joint on the HB-2B beam line at the Neutron Residual Stress Facility at HFIR. However, the neutron scattering to background noise ratio was very low during data acquisition. Measurements of lattice strains were obtained in the rolling (RD) and normal (ND) directions but not in the extrusion direction (ED) of the thin plate sample. Unfortunately, the quality of the data was not sufficient for determining the residual stresses in the butt joint. From the previous neutron scattering experiments conducted on four hot rolled plates (R1, R2, R3 and R4) of 14YWT, the residual stresses were calculated from lattice strain data and plotted in 2-D color contour maps for ED, RD and ND. The results showed variations in the magnitude and spatial position of residual stresses in the microstructure of the four plates. The magnitude in residual stresses in ED and RD increased gradually with increasing rolling deformation for R1 (50%) to R2 (76%), followed by larger increases in R3 (89%) and R4 (95%). The maximum peaks in residual stresses for R4 was ~710-730 MPa in ED and RD. The residual stresses in ND were below ~300 MPa for each of the 4 rolled plates, with a maximum residual stress in R4 (95%) of ~400 MPa. These results indicated that significant residual stresses representing ~57% of the yield stress of 14YWT (SM13) had accumulated in the 14YWT plate after hot rolling to the 1 mm thickness, which was used in the FSW experiments. The microstructure analysis of the 1.0 mm thick plate of 14YWT containing the butt joint produced by FSW revealed significant changes in the grain structure and texture between the unaffected zone (UZ) of the rolled plate and the butt joint weld. In the UZ, the grains were severely elongated after 95% deformation and mainly possessed the {101} texture component in the ED. Two predominant grain misorientation angles were observed: one consisting of small misorientations of <5º between highly elongated grains and the other consisting of large misorientations of >15º in pockets of small grains that might have formed by dynamic recrystallization processes during rolling of the plate at 1000ºC. The morphology and texture of grains in the heat affected zone (HAZ) were similar to those in UZ, except the grains had coarsened due to excess heat input during FSZ. A population of pores formed and the grains both coarsened and changed to isotropic morphology in the microstructure of the butt joint on both the advancing and retreating sides. The texture of grains in both regions were randomly orientated between the 3 poles {001}, {101} and {111}. The main difference in texture of grains between the advancing side and retreating side was with the misorientation angles of neighboring grains. Most of the grains in the advancing side had misorientation angles of >5º indicating that these grains experienced recrystallization. On the retreating side, areas containing larger grains showed high misorientation angles of >15º compared to areas appearing as bands of grains with misorientation angles of <5º and between 5º-15º. Numerous small pockets of grains with low misorientation angles of <5º were distributed in the microstructure among the grains showing high misorientation angles of >15º. It was determined that the grains associated with low misorientation angles contained sub-grain structures, which was consistent with both recrystallization and recovery mechanisms for grains located on the retreating side of the butt joint. These results demonstrate the complex microstructure that evolves in the microstructure of 14YWT resulting from the input of high temperatures and severe deformations during FSW.

36 MATERIALS SCIENCE↗

Valence, exchange interaction, and location of Mn ions in polycrystalline M n x G a 1 - x N ( x ≤ 0.04 )

In this paper, we present an experimental study for polycrystalline samples of the diluted magnetic semiconductor $\mathrm{M}{\mathrm{n}}_{x}\mathrm{G}{\mathrm{a}}_{1{-}x}\mathrm{N}(x{\le}0.04)$ in order to address some of the existing controversial issues. X-ray and neutron diffraction, x-ray absorption near-edge structure, and electron paramagnetic resonance experiments were used to characterize the structural, electronic, and magnetic properties of the samples, and inelastic neutron scattering was employed to determine the magnetic excitations associated with Mn monomers and dimers. Our main conclusions are as follows: (i) The valence of the Mn ions is $2+$. (ii) The $\mathrm{M}{\mathrm{n}}^{2+}$ ions experience a substantial single-ion axial anisotropy with parameter D = 0.027(3) meV. (iii) Nearest-neighbor $\mathrm{M}{\mathrm{n}}^{2+}$ ions are coupled antiferromagnetically. Finally, the exchange parameter $J={-}0.140(7)\mathrm{meV}$ is independent of the Mn content $x$; i.e., there is no evidence for hole-induced modifications of $J$ towards a potentially high Curie temperature postulated in the literature.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Nonstereotypical Distribution and Effect of Ergosterol in Lipid Membranes

Ergosterol, found in fungi and some protist membranes, is understudied compared with cholesterol from animal membranes. Generally, ergosterol is assumed to modulate membranes in the same manner as cholesterol, based on their similar chemical structures. Here we reveal some fundamental structural and dynamical differences between them. Neutron diffraction shows that ergosterol is embedded in the lipid bilayer much shallower than cholesterol. Further, ergosterol does not change the membrane thickness as much as cholesterol does, indicating little condensation effect. Neutron spin echo shows that ergosterol can rigidify and soften membranes at different concentrations. The lateral lipid diffusion measured by quasielastic neutron scattering indicates that ergosterol promotes a jump diffusion of the lipid, whereas cholesterol keeps the same continuous lateral diffusion as the pure lipid membrane. Our results point to quite distinct interactions of ergosterol with membranes compared with cholesterol. These insights provide a basic understanding of membranes containing ergosterol with implications for phenomena such as lipid rafts and drug interactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Perfect Crystals: microgravity capillary counterdiffusion crystallization of human manganese superoxide dismutase for neutron crystallography

The NASA mission Perfect Crystals used the microgravity environment on the International Space Station (ISS) to grow crystals of human manganese superoxide dismutase (MnSOD)—an oxidoreductase critical for mitochondrial vitality and human health. The mission’s overarching aim is to perform neutron protein crystallography (NPC) on MnSOD to directly visualize proton positions and derive a chemical understanding of the concerted proton electron transfers performed by the enzyme. Large crystals that are perfect enough to diffract neutrons to sufficient resolution are essential for NPC. This combination, large and perfect, is hard to achieve on Earth due to gravity-induced convective mixing. Capillary counterdiffusion methods were developed that provided a gradient of conditions for crystal growth along with a built-in time delay that prevented premature crystallization before stowage on the ISS. Here, we report a highly successful and versatile crystallization system to grow a plethora of crystals for high-resolution NPC.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Top Loading Helium Cryostat Integrated with High-Pressure Cell with Fast Remote Pressure Control (Final Report for SBIR Phase 1)

A large number of physical phenomena, such as superconductivity and quantum critical phenomena, often appear only at very low temperatures below 5 K. There is an immense interest to investigate these phenomena at high pressure as a means of tuning interatomic distances, and thus the interaction parameters controlling these phenomena, in a continuous and controlled fashion. The current P-T condition for neutron scattering experiments are limited to either relatively low pressures of about 2 GPa at temperatures below 5 K, or to relatively high temperatures at pressures or tens of GPa. The purpose of this research is to develop neutron sample environment instrumentation for reaching 10-20 GPa at 1-2K with rapid and reliable online pressure and temperature control (i.e. without having to interrupt the experiment). The ultimate goal of the project is to design an integrated fast-cooling low-temperature sample environment cryogenic system compatible with state of the art neutron diamond anvil cells suitable for single-crystal neutron scattering experiments for temperatures down to 2K and pressures of several tens of GPa. The integrated system will consist of top-loading Helium flow cryostat with in-situ sample alignment mechanisms, large-volume diamond anvil cells (DAC) made from novel superalloy Pascalloy and optimized for fast cooling and heating, and a compact remote pressure control mechanism for the DAC based on a novel concept of inflatable bellows integrated with a lever-arm based force amplifier. In Phase I, we have designed, manufactured, and tested prototypes of the novel compact force-amplified pneumatic pressure control mechanism for Neutron Diamond Anvil Cell (nDAC), which allows to use pneumatic bellows system for smooth remote pressure control in the nDAC inside a top-loading cryostat with bore size of 70 mm or larger. This allows significant minimum temperature decrease in remotely controlled nDAC from 5-10 K down to 2 K. We also studied mechanical properties of a novel non-magnetic superalloy Pascalloy with different heat-treatment conditions and preliminary results indicate that up to date this is probably the strongest and most suitable material for making more compact and lightweight cryogenic nDACs for neuron scattering experiments at extreme conditions, allowing much faster cooling and heating. Potential applications: The new developments will allow to create a wide range of compact Diamond Anvil Cells for neutron diffraction which can reach several tens of GPA pressure at 2-4 K while preserving accurate remote pressure control capabilities. The new concepts can be used for developing sample environment instrumentation outside the neutron scattering field. The new development have very strong potential for expanding experimental capabilities in materials sciences and have high commercialization potential. The proposed new cryogenic high-pressure system or any of its individual components will be in high demand not only in neutron scattering facilities, but also at synchrotron beamlines and other high-pressure research facilities around the world.

36 MATERIALS SCIENCE↗

Quantitative Uncertainty Analysis for Diffraction

Current software uses a least squares statistical method. For each model parameter, current software yields a point estimate and estimated standard error for each point estimate. In contrast, we have employed a Bayesian approach with sampling algorithm to provide a full posterior probability density function on each model parameter. This yields a different type of solution (probabilistic) with better fidelity. The Quantitative Uncertainty Analysis for Diffraction (QUAD) package returns a matrix of affect model parameters as a function of iteration through the MCMC analysis. QUAD is a Python code that allows for analysis of X-ray and neutron diffraction data to infer the structure of materials with quantifiable certainty. The code uses Bayesian statistics and Markov chain sampling algorithms to create posterior probability distributions on all material structure parameters that are modeled by a researcher. The statistical packages use the open source GSASII project as a library to calculate model diffraction patterns.

Fancher, ChristopherM↗

Crystal-field states and defect levels in candidate quantum spin ice Ce 2 Hf 2 O 7

Here, we report the synthesis of powder and single-crystal samples of cerium pyrohafnate and their characterization using neutron diffraction, thermogravimetry and x-ray absorption spectroscopy. We evaluate the amount of nonmagnetic Ce 4+ defects and use this result to interpret the spectrum of crystal-electric field transitions observed using inelastic neutron scattering. The analysis of these single-ion transitions indicates the dipole-octupole nature of the ground-state doublet and a significant degree of spin-lattice coupling. The single-ion properties calculated from the crystal-electric field parameters obtained spectroscopically are in good agreement with bulk magnetic susceptibility data down to about 1 K. Below this temperature, the behavior of the magnetic susceptibility indicates a correlated regime without showing any sign of magnetic long-range order or freezing down to 0.08 K. We conclude that Ce 2 Hf 2 O 7 is another candidate to investigate exotic correlated states of quantum matter, such as the octupolar quantum spin ice recently argued to exist in the isostructural compounds Ce 2 Sn 2 O 7 and Ce 2 Zr 2 O 7 .

36 MATERIALS SCIENCE↗

Phase diagram and spectroscopic signatures of a supersolid in the quantum ising magnet K 2 Co(SeO 3 ) 2

Supersolid phases are quantum-entangled states of matter exhibiting the dual characteristics of superfluidity and solidity. Theory predicts that hard-core bosons on a triangular lattice can form such phases at half filling and near complete filling. Leveraging an exact mapping between bosons and spin-$\frac{1}{2}$ degrees of freedom, here we show that these phases are realized in the triangular-lattice antiferromagnet K 2 Co(SeO 3 ) 2 . At zero field, neutron diffraction reveals the development of quasi-two-dimensional $\sqrt3$ x $\sqrt3$ magnetic order with Z 3 translational symmetry breaking (solidity), though with reduced amplitude indicating strong quantum fluctuations. These fluctuations manifest as equidistant bands of continuum neutron scattering, where the lowest-energy mode is gapless at K ($\frac{1}{3}$ $\frac{1}{3}$), consistent with broken U(1) spin rotational symmetry (superfluidity). For c-axis-oriented magnetic fields near saturation, we find a second phase consistent with a high-field supersolid. These two supersolids are separated by a pronounced 1/3 magnetization plateau phase that supports coherent spin waves, from which we determine the underlying spin Hamiltonian.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A compact in situ polarized 3He neutron spin filter for the diffractometer VULCAN at the Spallation Neutron Source

We have built and commissioned a compact in situ 3He polarizer based on spin-exchange optical pumping for the engineering materials diffractometer, named VULCAN, at the Spallation Neutron Source (SNS) at Oak Ridge National Laboratory. The system achieved 78% 3He polarization with a short pump-up time constant of 2.2 h. Its first deployment in an in situ half-polarized neutron diffraction experiment on a magnetic shape memory alloy, Ni–Mn–Ga, revealed changes in magnetization coupled to deformation twinning under compression. With this new capability, VULCAN has become the first diffractometer at SNS capable of performing polarized neutron experiments, opening new opportunities to study a wider range of magnetism-related material behaviors under varied thermal, mechanical, electrical, and/or magnetic fields.

Fu, Sichao [ORNL] (ORCID:0009000846771640)↗