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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 1,261 records · Page 70
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Unraveling the adsorption-limited hydrogen oxidation reaction at palladium surface via in situ electron microscopy

Palladium (Pd) catalysts have been extensively studied for the direct synthesis of H 2 O through the hydrogen oxidation reaction at ambient conditions. This heterogeneous catalytic reaction not only holds considerable practical significance but also serves as a classical model for investigating fundamental mechanisms, including adsorption and reactions between adsorbates. Nonetheless, the governing mechanisms and kinetics of its intermediate reaction stages under varying gas conditions remain elusive. This is attributed to the intricate interplay between adsorption, atomic diffusion, and concurrent phase transformation of catalyst. Herein, the Pd-catalyzed, water-forming hydrogen oxidation is studied in situ, to investigate intermediate reaction stages via gas cell transmission electron microscopy. The dynamic behaviors of water generation, associated with reversible palladium hydride formation, are captured in real time with a nanoscale spatial resolution. Our findings suggest that the hydrogen oxidation rate catalyzed by Pd is significantly affected by the sequence in which gases are introduced. Through direct evidence of electron diffraction and density functional theory calculation, we demonstrate that the hydrogen oxidation rate is limited by precursors’ adsorption. These nanoscale insights help identify the optimal reaction conditions for Pd-catalyzed hydrogen oxidation, which has substantial implications for water production technologies. The developed understanding also advocates a broader exploration of analogous mechanisms in other metal-catalyzed reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Shapes of rotating normal fluid He-3 versus superfluid He-4 droplets in molecular beams

Previous single-pulse extreme ultraviolet and X-ray coherent diffraction studies revealed that superfluid 4He droplets obtained in free jet expansion acquire sizable angular momentum, resulting in significant centrifugal distortion. Similar experiments with normal fluid 3He droplets may help elucidating the origin of the of the large degree of rotational excitation and highlight similarities and differences of dynamics in normal and superfluid droplets. Here, we present the first comparison of the shapes of isolated 3He and 4He droplets following expansion of the corresponding fluids in vacuum at temperatures as low as ~ 2 K. Large 3He and 4He droplets with average radii of ~160 nm and ~350 nm, respectively, were produced. We find that the majority of the 3He droplets in the beam correspond to rotating oblate spheroids with reduced average angular momentum ($\Lambda$) and reduced angular velocities ($\Omega$) similar to that of 4He droplets. Given the different physical nature of 3He and 4He, this similarity in $\Lambda$ and $\Omega$ may be surprising and suggest that similar mechanisms induce rotation regardless of the isotope. We hypothesized that the observed distribution of droplet sizes and angular momenta stem from processes in the dense region close to the nozzle. In this region, the significant velocity spread and collisions between the droplets induce excessive rotation followed by droplet fission. The process may repeat itself several times before the droplets enter the collision-fee high vacuum region further downstream.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Single-shot spatiotemporal plasma density measurements with a chirped probe pulse

In this work, we present the development and demonstration of a diagnostic for the measurement of the spatial and temporal evolution of plasma density in a single shot. Single-shot Advanced Plasma Probe HolographIc REconstruction (SAPPHIRE) utilizes a chirped probe pulse, a diffractive optical element, a self-referenced interferometer, and an interference bandpass filter to achieve high-fidelity electron density measurements suitable for underdense plasmas that exhibit cylindrical symmetry. The method overcomes limitations in conventional diagnostics, such as reliance on shot-to-shot reproducibility, while capturing plasma dynamics on picosecond timescales with micron-level spatial resolution. The capabilities of SAPPHIRE are demonstrated through measurements of laser-driven plasma channels in helium–nitrogen gas jets. SAPPHIRE demonstrates the formation and expansion of plasma channels in a single shot and the propagation of supersonic ionization fronts while revealing shot-to-shot variations in the plasma profiles. Experimental results are validated against theoretical models and scaling laws, underscoring the robustness and accuracy of this technique. By enabling ultrafast, high-resolution plasma diagnostics in a single exposure, SAPPHIRE represents a transformative advancement in plasma measurement technology.

Grace, Elizabeth S. [Lawrence Livermore National L↗
DOE OSTI2018

Quantifying the inter- and intra-granular stresses and their effects on deformation behaviors for the polycrystalline hexagonal beryllium by neutron diffraction

Highlights: • The inter- and intra-granular stresses are quantified for the polycrystalline hexagonal metal beryllium. • Composite behavior of the internal stresses is revealed in the polycrystalline beryllium. • Those internal stresses show the obvious grain-orientation dependence. • Those stresses can be significantly tuned by the temperature and strain rate effects. • The dislocation slip and twinning are quantified together with the inter- and intra-granular stored energies. - Abstract: The internal stresses developing at different length scales play the important role in materials performance. This importance has been well recognized for the cubic metals, however, not for the hexagonal close-packed (hcp) ones. The present work investigates the intergranular and intragranular stresses in the polycrystalline hexagonal beryllium by neutron diffraction. The correlation between those internal stresses and the deformation mechanism is revealed, and the strain rate and temperature effects on those stresses are presented. A composite behavior of intergranular and intragranular stresses is observed, which can be significantly tuned by the temperature and strain rate effects. The intergranular stress and stored energy are large for the soft-oriented grains (SOGs), while the intragranular stress and stored energy are large for the hard-oriented ones (HOGs). Both of those stresses are significantly high for the dynamic strain rate while they are relatively low for the elevated temperature. The large internal stresses in the dynamically compressed specimen should be attributed to the large number of twins and high density of dislocations. Different HOGs-SOGs configurations are proposed on the light of those observations, which might facilitate the properties controlling and extend the application scope for the hcp metal beryllium.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Lowering the Activation Barriers for Lithium-Ion Conductivity through Orientational Disorder in the Cyanide Argyrodite Li6PS5CN

Rapid advancements in safe and high-energy-density energy storage are predicated on identifying new solid-state ion conductors with low activation energies and high ionic conductivities for all-solid-state battery technologies. Halide argyrodites are among some of the top candidates for solid-state electrolytes, as they can achieve ionic conductivities that approach liquid electrolytes. Incorporating dynamic pseudohalide species in argyrodite solid electrolytes presents an exciting opportunity to exploit lattice dynamics as a design principle to modulate the ion conduction properties of solid-state ion conductors. In the present study, we have prepared the new argyrodite Li 6 PS 5 CN containing orientationally disordered cyanide ions. The new cyanide argyrodite Li 6 PS 5 CN exhibits an activation barrier to Li-ion transport of 471 ± 25 meV and a room-temperature ionic conductivity of 6(2) × 10 –5 S cm –1 in comparison to the activation barrier of 502 ± 16 meV and an ionic conductivity of 2.3(1) × 10 –4 S cm –1 measured for the bromide analogue Li 6 PS 5 Br. Structural studies of both compounds by high-resolution X-ray diffraction indicate that Li 6 PS 5 CN and Li 6 PS 5 Br adopt nearly identical crystal structures with similar lattice parameters, which indicates that lower activation barriers in Li 6 PS 5 CN arise due to the cyanide ion itself rather than due to changes in the geometry of conduction pathways in the local lithium environment. The orientational disorder of the quadrupolar cyanide ion in Li 6 PS 5 CN points to a complex interplay of lattice polarizability and molecular dynamics that lower the activation barrier for lithium-ion conductivity in the cyanide argyrodite.

25 ENERGY STORAGE↗
DOE OSTI2020

Failure investigation of nuclear grade POCO graphite target in high energy neutrino physics through numerical simulation

In many high energy physics neutrino beamlines, targets are made up of isotropic POCO graphite grade for production of neutrinos for high energy particle physics research and are bombarded with highly energetic pulsed proton beam. The pulsed proton beam with a small beam size creates thermal stress waves as well as radiation damage such as displacement damage, void formation, swelling, and gas formation amongst others. As a result, after a few years of operation one of the longest operated targets appears to have undergone bulk swelling and fractured along the beam centerline. A complex interaction of dynamic loading due to beam, material degradation due to irradiation are thought to have caused such a failure. Here, we present a numerical simulation to capture the combined effects of swelling and the dynamic effect of thermal stress waves due to beam heating, to explain the failure of target. An empirical formula has been developed to take into account swelling as a function of temperature and proton fluence and has been implemented in a commercial finite element code. Extensive X-ray diffraction (XRD) were performed on graphite samples from the failed target to understand the lattice parameter changes due to irradiation and build a valid empirical model. Simulation results show that swelling plays a major role in elevating the stress state in the material exceeding the failure strength while the pulsed beam heating also introduces fatigue loading that would explain brittle fracture emanating from inside of the material and propagating outward. Such empirical formulations will help in identifying the threshold values of critical parameters to extend the service life of future multi-megawatt neutrino targets and targets in other accelerator environments.

43 PARTICLE ACCELERATORS↗
DOE OSTI2018

Active site localization of methane oxidation on Pt nanocrystals

High catalytic efficiency in metal nanocatalysts is attributed to large surface area to volume ratios and an abundance of under-coordinated atoms that can decrease kinetic barriers. Although overall shape or size changes of nanocatalysts have been observed as a result of catalytic processes, structural changes at low-coordination sites such as edges, remain poorly understood. Here in this paper, we report high-lattice distortion at edges of Pt nanocrystals during heterogeneous catalytic methane oxidation based on in situ 3D Bragg coherent X-ray diffraction imaging. We directly observe contraction at edges owing to adsorption of oxygen. This strain increases during methane oxidation and it returns to the original state after completing the reaction process. The results are in good agreement with finite element models that incorporate forces, as determined by reactive molecular dynamics simulations. Reaction mechanisms obtained from in situ strain imaging thus provide important insights for improving catalysts and designing future nanostructured catalytic materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Photoinduced evolution of lattice orthorhombicity and conceivably enhanced ferromagnetism in LaMnO 3 membranes

Ultrashort laser pulses have been utilized to dynamically drive phase transitions in correlated quantum materials. Of particular interest is whether phases not achievable in thermal equilibrium can be induced in complex oxides with intricately coupled lattice, electron and spin degrees of freedom. Here, we tracked atomic motions in LaMnO 3 following photoexcitation with MeV ultrafast electron diffraction (MeV-UED) technique. We found that the light excited state exhibits numerous signatures different from thermal equilibrium ones, including nearly conserved Bragg intensities, strongly suppressed La cation and oxygen anion displacements, and the long-range lattice orthorhombicity evolution. Furthermore, using first-principles calculations, we predict that the ferromagnetic ordering and conductivity are both enhanced upon laser excitation due to the reduction of the lattice orthorhombicity. This work benefits from recent advance in fabrication of membrane films with high epitaxial quality and in MeV-UED with large momentum space access and high temporal resolution.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Constraining the release of Sn to the ambient melting point following shock loading using time-resolved x-ray diffraction

The formation of liquid following release from a shocked state governs the transition from spall to cavitation and the formation of ejecta in metals. In order to build physics-based models of these processes, it is necessary to critically evaluate the relative importance of kinetics and entropy generation during the release along with the accuracy of multiphase equations of state. Tin (Sn) has served as a testbed for a variety of experiments examining strength and ejecta due to its accessible melt boundary and solid–solid phase transitions. This work presents experiments examining the phase evolution of high purity Sn following the shock and release to ambient stress near the melting point. Sn is found to release to states between its ambient solidus and liquidus from approximately 19 to 33 GPa under uniaxial loading, with the two-phase region being characterized by a reduction in the intensity of the (220), (211) β -Sn doublet. Jetting experiments performed at 27–28 GPa exhibit comparable diffraction patterns with what is observed following the uniaxial release. The solid fractions of β-Sn in the ambient mixed phase region are found to decrease linearly with increasing shock stress as increasing liquid Sn is formed. Here, the results provide much needed information for interpreting measurements of dynamic strength at a high strain rate and experiments examining cavitation and shallow bubble collapse in Sn.

, spall↗
DOE OSTI2020

Temperature-dependent kinetic pathways featuring distinctive thermal-activation mechanisms in structural evolution of ice VII

Significance The kinetics of the structural evolution from crystalline ice (ice VII or ice VIII) toward thermodynamically stable ice I at ambient pressure have been characterized using time-resolved in situ X-ray diffraction. The time resolution captures events that were not observed previously and reveals a complex kinetic pathway with three distinctive transitions, i.e., amorphization, amorphous–amorphous, and crystallization of amorphous ice into ice I. The first two transitions exhibit different thermally activated mechanism above and below 110 K. Molecular-dynamics simulations show the transition involves a large change in density and substantial displacements of water at the nanoscale. This study presents a perspective on the metastability and complexity of the energy landscape in temperature/time-dependent structural evolution in amorphous ices.

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

Polymorphism of gold under laser-based ramp compression to 690 GPa

The high-pressure behavior and polymorphism of gold has attracted strong recent interest from theory as well as from both static and dynamic experiments. In this study, gold was dynamically ramp-compressed to 690 GPa via laser ablation using the Omega Laser Facility (U. Rochester) in order to investigate the stability regions of this noble metal's polymorphs. Here, stresses were determined from measurements of surface or interface velocities by laser interferometry. In situ X-ray diffraction was carried out to constrain the structure and density. The ambient face-centered-cubic (fcc) phase was observed at 162 GPa, followed by a mixed phase region consisting of the fcc and body-centeredcubic (bcc). The presence of only the bcc phase was observed between 377 and 690 GPa. Our results are consistent with recent shock compression experiments and demonstrate that gold transforms to the bcc phase under conditions of both ramp and shock loading.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

From Ising Resonant Fluctuations to Static Uniaxial Order in Antiferromagnetic and Weakly Superconducting CeCo ( In 1 - x Hg x ) 5 ( x = 0.01 )

CeCo (In 0.990 Hg 0.010 ) 5 is a charge doped variant of the d-wave CoCoIn 5 superconductor with coexistent antiferromagnetic and superconducting transitions occurring at T N = 3.4 and T c = 1.4 K, respectively. We use neutron diffraction and spectroscopy to show that the magnetic resonant fluctuations present in the parent superconducting phase are replaced by collinear c -axis magnetic order with three-dimensional Ising critical fluctuations. No low-energy transverse spin fluctuations are observable in this doping-induced antiferromagnetic phase and the dynamic resonant spectral weight predominately shifts to the elastic channel. Static (τ > 0.2 ns) collinear Ising order is proximate to superconductivity in CeCoIn 5 and is stabilized through hole doping with Hg.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Second Target Station (STS) Project: Centaur (Technical Report)

CENTAUR will be the flagship general purpose small-angle neutron scattering (SANS) instrument for the Second Target Station of SNS. Based on an optimized and high-performance SANS instrument, it is capable of SANS/wide-angle neutron scattering and diffraction simultaneously filling the capability gap to cover structure scale from atomic scale to hundreds of nanometers for scientific needs ranging from polymers, biology, materials sciences, and quantum condensed matter. Additionally, with a high-speed chopper, it can be used as a direct geometry spectrometer to probe the dynamics in relatively large length-scale structures as an inelastic SANS spectrometer. The technical details of the CENTAUR instrument are presented in this document. As the project progresses, the initial details are subject to change based on feedback.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2016

In situ high-energy X-ray diffraction study of tensile deformation of neutron-irradiated polycrystalline Fe-9%Cr alloy

The effect of neutron irradiation on tensile deformation of a Fe-9wt.%Cr alloy was investigated using in situ high-energy synchrotron X-ray diffraction during room-temperature uniaxial tensile tests. New insights into the deformation mechanisms were obtained through the measurements of lattice strain evolution and the analysis of diffraction peak broadening using the modified Williamson-Hall method. Two neutron-irradiated specimens, one irradiated at 300 °C to 0.01 dpa and the other at 450 °C to 0.01dpa, were tested along with an unirradiated specimen. The macroscopic stress–strain curves of the irradiated specimens showed increased strength, reduced ductility and work-hardening exponent compared to the unirradiated specimen. The evolutions of the lattice strain, the dislocation density and the coherent scattering domain size in the deformation process revealed different roles of the submicroscopic defects in the 300°C/0.01 dpa specimen and the TEM-visible nanometer-sized dislocation loops in the 450°C/0.01 dpa specimen: submicroscopic defects extended the linear work hardening stage (stage II) to a higher strain, while irradiation-induced dislocation loops were more effective in dislocation pinning. Lastly, while the work hardening rate of stage II was unaffected by irradiation, significant dynamic recovery in stage III in the irradiated specimens led to the early onset of necking without stage IV as observed in the unirradiated specimen.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Structural and Reorientational Dynamics of Tetrahydroborate (BH4-) and Tetrahydrofuran (THF) in a Mg(BH4)2 3THF Adduct: Neutron-Scattering Characterization

Metal borohydrides are considered promising materials for hydrogen storage applications due to their high volumetric and gravimetric hydrogen density. Recently, different Lewis bases have been complexed with Mg(BH4)2 in efforts to improve hydrogenation/dehydrogenation properties. Notably, Mg(BH4)2 xTHF adducts involving tetrahydrofuran (THF; C4H8O) have proven to be especially interesting. This work focuses on exploring the physicochemical properties of the THF-rich Mg(BH4)2 3THF adduct using neutron-scattering methods and molecular DFT calculations. Structural analysis, based on neutron diffraction measurements of Mg(11BH4)2 3TDF (D-deuterium), has confirmed a lowering of the symmetry upon cooling, from monoclinic C2/c to P[1 with combining macron] via a triclinic distortion. Vibrational properties are strongly influenced by the THF environment, showing a splitting in spectral features as a result of changes in the bond lengths, force constants, and lowering of the overall symmetry. Interestingly, the orientational mobilities of the BH4- anions obtained from quasielastic neutron scattering (QENS) are not particularly sensitive to the presence of THF and compare well with the mobilities of BH4- anions in unsolvated Mg(BH4)2. The QENS data point to uniaxial 180 degree jump reorientations of the BH4- anions around a preferred C2 anion symmetry axis. The THF rings are also found to be orientationally mobile, undergoing 180 degree reorientational jumps around their C2 molecular symmetry axis with jump frequencies about an order of magnitude lower than those for the BH4- anions. In contrast, no dynamical behavior of the THF rings is observed with QENS for a more THF-deficient 2Mg(BH4)2 THF adduct. This lack of comparable THF mobility may reflect a stronger Mg2+-THF bonding interaction for lower THF/Mg(BH4)2 stoichiometric ratios, which is consistent with DFT calculations showing a decrease in the binding energy with each additional THF ring in the adduct. Based on the combined experimental and computational results, we propose that combining THF and Mg(BH4)2 is beneficial to (i) preventing weakly bound THF from coming free from the Mg2+ cation and reducing the concentration of any unwanted impurity in the hydrogen and (ii) disrupting the stability of the crystalline phase, leading to a lower melting point and enhanced kinetics for any potential hydrogen storage applications.

36 MATERIALS SCIENCE↗