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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

First Examination of Irradiated Fuel with Pulsed Neutrons at LANSCE (Preliminary Results)

We present preliminary results on the characterization of an irradiated U-lOZr-lPd fuel sample that was prepared from the irradiated AFC-3A-R5A sample. U-lOZr metallic fuels are researched as host materials for potential transmutation fuels and the addition of palladium strives to bind lanthanides, thus preventing fuel-cladding chemical interactions (FCCI). These interactions limit the lifetime of metallic fuels and are caused by migration of lanthanide fission products to the periphery of the fuel slug, where they start to interact with the D9 or HT9 steel cladding, ultimately leading to failure of the mechanical integrity of the cladding. Neutrons offer bulk characterization of irradiated materials for which X-ray tomography methods are not suitable due to the immense gamma background emitted from the samples. In particular pulsed neutrons provide information from the ability to resolve the neutron energy using their time-of-flight and thus the potential to utilize neutron absorption resonance to characterize the spatial distribution of isotopes. This, in turn, may allow to characterize the distribution of fission and neutron capture products non-destructively and may ultimately be applied to the bulk of an irradiation capsule prior to destructive post-irradiation examination to identify regions of interest. To allow the characterization of entire irradiation capsules, a cask is under development in the advanced post-irradiation work package at LANL and progress on this development was reported elsewhere. In parallel, an irradiated U-lOZr-lPd sample cut from the AFC-3AR5A irradiation was shipped to LANL and will be fully characterized with an NSUF funded rapid turnaround experiment (RTE) in the 2020 LANSCE run cycle. The sample emits at a dose rate of ~3R/hr on contact and is therefore manageable with remote handling, without requiring a cask. The disk-shaped material is larger than samples prepared for analysis using electron or X-ray methods and is therefore an intermediate step towards characterization of bulk samples at LANSCE. However, since it covers the full diameter of the irradiated fuel slug, some insight on redistribution of elements, spatially resolved information on microstructure, e.g. phase composition and texture, will be possible using the pulsed neutron-based methods developed for fuel characterization at LANSCE. This report describes the development of procedures to handle the sample at LANSCE as well as preliminary data and results from tests conducted in December 2019 on the energy-resolved neutron imaging (ERNI) beam line at flight path 5 and the high pressure-preferred orientation diffractometer (HIPPO) at LANSCE. This effort is a collaboration between LANL, INL, and ORNL. To compare our capabilities with prior work, we present an overview of previously reported bulk characterization of irradiated or spent fuels. The overview addresses neutron diffraction and neutron absorption resonance spectroscopy, both of which have only few reported applications on irradiated or spent nuclear fuel, as well as neutron radiography. This literature review was already described in a previous report but is repeated here to put our current efforts in context of previous work.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Cation Dynamics in Hybrid Halide Perovskites

Hybrid halide perovskite semiconductors exhibit complex, dynamical disorder while also harboring properties ideal for optoelectronic applications that include photovoltaics. However, these materials are structurally and compositionally distinct from traditional compound semiconductors composed of tetrahedrally coordinated elements with an average valence electron count of silicon. The additional dynamic degrees of freedom of hybrid halide perovskites underlie many of their potentially transformative physical properties. Neutron scattering and spectroscopy studies of the atomic dynamics of these materials have yielded significant insights into their functional properties. Specifically, inelastic neutron scattering has been used to elucidate the phonon band structure, and quasi-elastic neutron scattering has revealed the nature of the uncorrelated dynamics pertaining to molecular reorientations. Understanding the dynamics of these complex semiconductors has elucidated the temperature-dependent phase stability and origins of defect-tolerant electronic transport from the highly polarizable dielectric response. Furthermore, the dynamic degrees of freedom of the hybrid perovskites provide additional opportunities for application engineering and innovation.

Materials Science↗
DOE OSTI2024

Enhancing Low-Temperature Syngas Production via Surface Tailoring of Supported Intermetallic Nanocatalysts

An active and coke-resistant silica-encapsulated intermetallic Ni 3 Zn nanoparticle catalyst was developed for low-temperature (450 °C) dry reforming of methane (DRM). The catalyst exhibited a remarkable 4-fold increase in activity (4.5 s –1 ) with over 99% CO selectivity and 3 orders of magnitude less carbonaceous species and demonstrated remarkable stability (70 h) compared to that of a monometallic Ni catalyst. Here, the key is the combined effect of surface ensemble structure and electronic interaction modulation through the surface composition tailoring achieved by off-stoichiometric Ni and Zn loading in controlling surface chemistry for achieving different activities and H 2 /CO ratios. Characterized by ion spectroscopy, X-ray photoelectron spectroscopy, and the neutron pair distribution function, it was revealed that paired Ni δ – –Zn δ+ active sites are crucial for DRM. Transient infrared spectroscopy and isotopic analysis uncovered the synergistic effect of Ni δ – –Zn δ+ sites in activating C–H bonds and dissociating CO 2 to prevent coke formation under low-temperature conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

15 years of spin-echo spectroscopy at SNS-NSE: Looking back and looking forward

High-resolution neutron spin echo (NSE) spectroscopy offers unique insights into the mobility of molecular (sub)structures excited by thermal fluctuations (i.e., Brownian motion) of “soft matter” as polymers in solution and in the melt, in biological matter (e.g., protein motions), membranes, and glasses. The ability to tag substructures using H, D contrast variation to resolve the relevant timescales of dynamics on selected molecular items in liquids, soft matter, and melts is a significant advantage of NSE. Also slow magnetic fluctuations on molecular length scales in the range of nanoseconds, e.g., in spin glasses or topological spin structures, can be accessed. This paper reviews the highlights and peculiarities of the SNS-NSE, based at the pulsed neutron source SNS, during its first 1.5 decades of operation. An outlook and perspectives of research in the domain of high-resolution spectroscopy is given.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

First observation of a shape isomer and a low-lying strongly-coupled prolate band in neutron-deficient semi-magic 187 Pb

Prompt and delayed gamma-ray spectroscopy of the neutron-deficient, semi-magic isotope 187Pb has been performed using the recoil-decay and isomer-decay tagging techniques at the Argonne Gas-Filled Analyzer. A new 5.15(15)-mu s isomeric state at only 308 keV above the spherical 3/2 - ground state is identified and classified as a shape isomer. A strongly-coupled band is observed on top of the isomer, which is nearly identical to the one built on the prolate 7/2 - [514] Nilsson state in the isotone 185 Hg. Based on this similarity and on the result of the potential-energy surface calculations, the new isomer in 187 Pb is proposed to originate from the same configuration. The retarded character of the 308-keV (7/2( - )→ 3/2$_{gs}^{-}$ transition with a deduced B(E2) = 5.6(2) x 10 -4 W.u. can be well explained by the significant difference between the prolate parent and spherical daughter configurations, leading to the shape isomerism. The excitation energy of the isomer is surprisingly low, being roughly half of the excitation energies of the known 0 + intruder bandheads in the neighboring 186,188 Pb isotopes. The combined results of the present work and the previous alpha-decay and laser spectroscopy studies present evidence for triple shape coexistence at low energy in the negative-parity configurations of 187 Pb, which is well reproduced by the potential-energy surface calculations.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Influence of Grafting Density and the Ionic Environment on the Structure of Zwitterionic Brushes

Zwitterionic polymer brushes possess a high potential for applications as surface coatings, e.g., in antifouling applications. Their complex association behavior due to the coexistence of oppositely charged groups on the same monomeric unit allows for a broad variation of polarity, hydrophilicity, and the antipolyelectrolyte effect with the variation of the surrounding environment. In this study, planar polysulfobetaine brushes were investigated with neutron reflectometry (NR) and neutron spin–echo spectroscopy under grazing incidence (GINSES) to explore the brush structure and its inner dynamics perpendicular to the substrate. In particular, the effects of the substrate–initiator system and ionic strength on the structure were investigated with neutron reflectometry and a swelling by a factor of 3–5 was found in the presence of aqueous NaCl and MgCl 2 solutions compared to the dry state. During the data analysis, the applicability of a model-free evaluation was also demonstrated for the investigated polysulfobetaine brushes. Furthermore, it was found with GINSES that in contrast to neutral brushes, these polysulfobetaine brushes do not show the typical concentration fluctuations in the nanosecond time range when partially swollen with salt-free water.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Exploring cesium properties internal to the LANSCE H - ion source using resonant absorption spectroscopy

The Los Alamos Neutron Science Center (LANSCE) H - ion source has provided stable output for decades of LANL mission needs, but its maximum beam output has remained the same at ~15 mA. A roadblock to improving beam output has been a lack of thorough understanding of the internal mechanisms of LANSCE H - ion source. The LANSCE H - Ion Source Laser Diagnostic Stand (HLDS) was recently built and commissioned to explore these internal mechanisms using laser absorption techniques, to measure and diagnose dynamic H - and cesium densities. The cesium density probe is based on resonant absorption of a continuous wave diode laser tuned though the D 2 line of cesium (~852 nm). The diagnostic capabilities of HLDS will be reviewed, and measurements using the cesium laser diagnostic will be presented.

43 PARTICLE ACCELERATORS↗
DOE OSTI2021

Investigation of glass-ceramic lithium thiophosphate solid electrolytes using NMR and neutron scattering

Solid-state Li batteries require solid electrolytes which have high Li+ conductivity and good chemical/mechanical compatibility with Li metal anodes and high energy cathodes. Structure/function correlations which relate local bonding to macroscopic properties are needed to guide development of new solid electrolyte materials. This study combines diffraction measurements with solid-state nuclear magnetic resonance spectroscopy (ssNMR) and neutron pair distribution function (nPDF) analysis to probe the short-range vs. long-range structure of glass-ceramic Li 3 PS 4 -based solid electrolytes. Here, we demonstrate how different synthesis conditions (e.g., solvent selection and thermal processing) affect the resulting polyanionic network. More specifically, structures with high P coordination numbers (e.g., PS 4 3– and P 2 S 7 4– ) correlate with higher Li + mobility compared to other polyanions (e.g., (PS 3 ) n n– chains and P 2 S 6 4– ). Overall, this work demonstrates how ssNMR and nPDF can be used to draw key structure/function correlations for solid-state superionic conductors.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Decay spectroscopy of 160 Eu: Quasiparticle configurations of excited states and structure of K π = 4 + bandheads in 160 Gd

Background: Detailed spectroscopy of neutron-rich, heavy, deformed nuclei is of broad interest for nuclear astrophysics and nuclear structure. Nuclei in the r-process path and following freeze-out region impact the resulting r-process abundance distribution, and the structure of nuclei midshell in both proton and neutron number helps to understand the evolution of subshell gaps and large deformation in these nuclei. Purpose: We aim to improve the understanding of the nuclear structure of 160 Gd, specifically the K π = 4 + bands, as well as study the β decay of 160 Eu into 160 Gd. Methods: High-statistics decay spectroscopy of 160 Gd resulting from the β-decay of 160 Eu was collected using the GRIFFIN spectrometer at the TRIUMF-ISAC facility. Results: Two new excited states and ten new transitions were observed in 160 Gd. The β-decaying half-lives of the low- and high-spin isomers in 160 Eu were determined, and the low-spin state's half-life was measured to be t 1/2 = 26.0 (8) s, ≈ 16% shorter than previous measurements. Lifetimes of the two K π = 4 + bandheads in 160 Gd were measured for the first time, as well as γ – γ angular correlations and mixing ratios of intense transitions out of those bandheads. Conclusions: Lifetimes and mixing ratios suggest that the hexadecapole phonon model of the K π = 4 + bandheads in 160 Gd is preferred over a simple two-state strong mixing scenario, although further theoretical calculations are needed to fully understand these states. Additionally, the 1999.0-keV state in 160 Gd heavily populated in β decay is shown to have positive parity, which raises questions regarding the structure of the high-spin β-decaying state in 160 Eu.

150 ≤ A ≤ 189↗
DOE OSTI2024

Microstructural Underpinnings of Giant Intrinsic Exchange Bias in Epitaxial NiCo 2 O 4 Thin Films

Understanding intrinsic exchange bias in nominally single-component ferromagnetic or ferrimagnetic materials is crucial for simplifying related device architectures. However, the mechanisms behind this phenomenon and its tunability remain elusive, which hinders the efforts to achieve unidirectional magnetization for widespread applications. Inspired by the high tunability of ferrimagnetic inverse spinel NiCo 2 O 4 , the origin of intrinsic exchange bias in NiCo 2 O 4 (111) films deposited on Al 2 O 3 (0001) substrates are investigated. The comprehensive characterizations, including electron diffraction, X-ray reflectometry and spectroscopy, and polarized neutron reflectometry, reveal that intrinsic exchange bias in NiCo 2 O 4 (111)/Al 2 O 3 (0001) arises from a reconstructed antiferromagnetic rock-salt Ni x Co 1-x O layer at the interface between the film and the substrate due to a significant structural mismatch. Remarkably, by engineering the interfacial structure under optimal growth conditions, it can achieve exchange bias larger than coercivity, leading to unidirectional magnetization. Such giant intrinsic exchange bias can be utilized for realistic device applications. This work establishes a new material platform based on NiCo 2 O 4 , an emergent spintronics material, to study tunable interfacial magnetic and spintronic properties.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Experimental determination of the temperature-dependent Van Hove function in a Zr 80 Pt 20 liquid

Even though the viscosity is one of the most fundamental properties of liquids, the connection with the atomic structure of the liquid has proven elusive. By combining inelastic neutron scattering with the electrostatic levitation technique, the time-dependent pair-distribution function (i.e., the Van Hove function) has been determined for liquid Zr 80 Pt 20 . We show that the decay time of the first peak of the Van Hove function is directly related to the Maxwell relaxation time of the liquid, which is proportional to the shear viscosity. This result demonstrates that the local dynamics for increasing or decreasing the coordination number of local clusters by one determines the viscosity at high temperature, supporting earlier predictions from molecular dynamics simulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Insights into the Rich Polymorphism of the Na + Ion Conductor Na 3 PS 4 from the Perspective of Variable-Temperature Diffraction and Spectroscopy

Solid electrolytes are crucial for next-generation solid-state batteries, and Na 3 PS 4 is one of the most promising Na + conductors for such applications, despite outstanding questions regarding its structural polymorphs. In this contribution, we present a detailed investigation of the evolution in structure and dynamics of Na 3 PS 4 over a wide temperature range 30 < T T < 500 °C, which we attribute to dynamic local tetragonal distortions. The first-order phase transition to the mesophasic high-temperature polymorph (γ, Fddd ) is associated with a sharp volume increase and the onset of liquid-like dynamics for sodium-cations (translational) and thiophosphate-polyanions (rotational) evident by inelastic neutron and Raman spectroscopies, as well as pair-distribution function and molecular dynamics analyses. Overall, these results shed light on the rich polymorphism of Na 3 PS 4 and are relevant for a range host of high-performance materials deriving from the Na 3 PS 4 structural archetype.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Biomembrane Structure and Material Properties Studied With Neutron Scattering

Cell membranes and their associated structures are dynamical supramolecular structures where different physiological processes take place. Detailed knowledge of their static and dynamic structures is therefore needed, to better understand membrane biology. The structure–function relationship is a basic tenet in biology and has been pursued using a range of different experimental approaches. In this review, we will discuss one approach, namely the use of neutron scattering techniques as applied, primarily, to model membrane systems composed of lipid bilayers. An advantage of neutron scattering, compared to other scattering techniques, is the differential sensitivity of neutrons to isotopes of hydrogen and, as a result, the relative ease of altering sample contrast by substituting protium for deuterium. This property makes neutrons an ideal probe for the study of hydrogen-rich materials, such as biomembranes. In this review article, we describe isotopic labeling studies of model and viable membranes, and discuss novel applications of neutron contrast variation in order to gain unique insights into the structure, dynamics, and molecular interactions of biological membranes. We specifically focus on how small-angle neutron scattering data is modeled using different contrast data and molecular dynamics simulations. We also briefly discuss neutron reflectometry and present a few recent advances that have taken place in neutron spin echo spectroscopy studies and the unique membrane mechanical data that can be derived from them, primarily due to new models used to fit the data.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

End block dynamics in unentangled polymers by dielectric spectroscopy

Dielectric spectroscopy measures the dynamics of polymer melts over a broad frequency range. Developing a theory for the spectral shape can extend the analysis of dielectric spectra beyond determining relaxation times from the peak maxima and adds physical meaning to shape parameters determined with empirical fit functions. Toward this goal, we use the experimental results on unentangled poly(isoprene), and unentangled poly(butylene oxide), polymer melts, to test whether the concept of end blocks could be one reason for the Rouse model deviating from experimental data. These end blocks have been suggested by simulations and neutron spin echo spectroscopy and are a consequence of the monomeric friction coefficient depending on the position of the bead in the chain. The concept of an end block is an approximation which partitions the chain in a middle and two end blocks to avoid overparameterization by a continuous position dependent change of the friction parameter. Analysis of dielectric spectra shows that the deviations of the calculated from the experimental normal mode cannot be related to the end block relaxation. However, the results do not contradict an end block hiding below the segmental relaxation peak. Finally, it seems that the results are compatible with an end block being the specific part of the sub-Rouse chain interpretation close to the chain ends.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Carbon Coating Influence on the Formation of Percolating Electrode Networks for Silicon Anodes

Previous studies have demonstrated that chemical vapor deposition carbon coating on silicon (Si@C) can enhance the electrochemical performance of lithium-ion batteries with Si-based anodes. However, the underlying mechanisms contributing to this improvement have not been fully explored. Here, we address this knowledge gap by applying a suite of characterization methods to evaluate Si@C anodes prepared by reducing acetylene on ball-milled Si particles. Raman mapping measurements show that the C coating (<5 nm thick) enables a homogeneous Si and carbon distribution during the slurry casting process, thereby promoting Si utilization during cycling. The coating’s microstructure and morphology were evaluated using X-ray photoelectron spectroscopy (XPS), scanning transmission electron microscopy, and neutron reflectivity experiments. Electrochemical impedance spectroscopy measurements upon cycling indicate that carbon coating also reduces the overall resistance as benchmarked against bare Si anodes. Galvanostatic cycling in half-cell studies revealed higher initial Coulombic efficiency and specific capacities with increasing carbon coating time. However, solid electrolyte interphase (SEI) investigations using XPS showed that the coated and uncoated samples have very similar characteristics, suggesting that the SEI may only play a minor role in enhancing the performance of Si@C. Full-cell evaluation of the Si electrodes was consistent with half-cell results relating to performance and SEI properties, further supporting the conclusion that electronic and ionic percolation, enabled by effective electrode manufacturing, are the dominant factors contributing to the favorable performance of Si@C.

25 ENERGY STORAGE↗
DOE OSTI2021

Intramolecular structure and dynamics in computationally designed peptide-based polymers displaying tunable chain stiffness

Here, polymers assembled using computationally designed coiled coil bundlemers display tunable stiffness via control of interbundlemer covalent connectivity as confirmed using small-angle neutron scattering. Neutron spin echo spectroscopy reveals that rigid rod polymers show a decay rate Γ~Q 2 (Q is the scattering vector) expected of straight cylinders. Semirigid polymers assembled using bundlemers linked via 4-armed organic linker show flexible segmental dynamics at mid-Q and Γ~Q 2 behavior at high Q. The results give insight into linker flexibility-dependent interbundlemer dynamics in the hybrid polymers.

36 MATERIALS SCIENCE↗