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At least 721 records · Page 40

Summary Statistics for LC_HT01_130808: Micro-CT Data Acquired at LLNL, Specimen 1 of 3

Using x-ray micro computed tomography (MicroCT), we have characterized the linear attenuation coefficients (LAC), μ, of a sample of a dry powder material, lithium carbonate (LC). The specimen was prepared at Lawrence Livermore National Laboratory (LLNL), loaded into a 60mL low density polyethylene (LDPE) bottle. After completed packing, the specimen was scanned following the protocol for MicroCT measurements under Test Plan 79. This particular specimen, LC_HT01_130808, recorded the bulk packing density (mass of sample divided by volume of sample) shown above. Two additional preparations were made and analyzed. We used the computer program IMGREC to reconstruct the CT images. The values of the key parameters used in the x-ray data capture and image reconstruction are given in this report. Additional experimental details may be found in the SOP and a separate document. To characterize the statistical distribution of LAC values in each CT image, we first isolated an ~80% region or segment of volume elements (“voxels”) lying completely within the sample, away from the walls of the container. We then calculated the mean value, standard deviation and entropy for (a) the high and low energy image segments and for (b) their digital gradient images. The statistics of the initial image of LAC values are called “first order statistics;” those of the gradient image, “second order statistics.” See Seetho for details of the analysis used to obtain the numbers reported in this document.

42 ENGINEERING↗

Liquid lithium wetting and percolation in a porous tungsten/liquid Li plasma facing component (PFC)

This work explores the concept of a hybrid material system designed to protect the plasma from high-Z material emission while also protecting an underlying high-Z wall material from erosion by integrating a low-Z component in the liquid phase. Plasma-surface interaction properties of a porous tungsten (W)-liquid metal hybrid system, having the favorable bulk thermomechanical properties of W while serving as a scaffold for a liquid metal with self-healing and radiative vapor shielding characteristics, are examined. W-substrates with 70% density of bulk W and 1–5 μm sized pores have been fabricated with 50-nm W powders using spark plasma sintering. Enhanced lithium (Li) wettability, driven by percolation through the porous W architecture, is demonstrated with in-situ liquid Li drop measurements. Finally, results show complete wetting of liquid Li at 250 °C in the porous W, 100 °C lower temperature than what has been observed on traditional W surfaces. In operando ion beam analysis of Li films deposited on porous W substrates provides microscopic evidence of Li percolation into the substrate and a first look at D retention up to a depth of 100 nm after plasma exposure at a flux of 10 20 m –2 s –1 , 250 eV/amu D + plasma to a fluence of 1.16 × 10 23 m –2 at a temperature of 200 °C.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Investigating the architecture and internal structure of the TOI-561 system planets with CHEOPS, HARPS-N, and TESS

ABSTRACT We present a precise characterization of the TOI-561 planetary system obtained by combining previously published data with TESS and CHEOPS photometry, and a new set of 62 HARPS-N radial velocities (RVs). Our joint analysis confirms the presence of four transiting planets, namely TOI-561 b (P = 0.45 d, R = 1.42 R⊕, M = 2.0 M⊕), c (P = 10.78 d, R = 2.91 R⊕, M = 5.4 M⊕), d (P = 25.7 d, R = 2.82 R⊕, M = 13.2 M⊕), and e (P = 77 d, R = 2.55 R⊕, M = 12.6 R⊕). Moreover, we identify an additional, long-period signal (>450 d) in the RVs, which could be due to either an external planetary companion or to stellar magnetic activity. The precise masses and radii obtained for the four planets allowed us to conduct interior structure and atmospheric escape modelling. TOI-561 b is confirmed to be the lowest density (ρb = 3.8 ± 0.5 g cm−3) ultra-short period (USP) planet known to date, and the low metallicity of the host star makes it consistent with the general bulk density-stellar metallicity trend. According to our interior structure modelling, planet b has basically no gas envelope, and it could host a certain amount of water. In contrast, TOI-561 c, d, and e likely retained an H/He envelope, in addition to a possibly large water layer. The inferred planetary compositions suggest different atmospheric evolutionary paths, with planets b and c having experienced significant gas loss, and planets d and e showing an atmospheric content consistent with the original one. The uniqueness of the USP planet, the presence of the long-period planet TOI-561 e, and the complex architecture make this system an appealing target for follow-up studies.

Lacedelli, G. (ORCID:0000000241977374)↗

The basis for reevaluating the reactivity of pyrite surfaces: spin states and crystal field d-orbital splitting energies of bulk, terrace, edge, and corner Fe( II ) ions

Pyrite, one of the most important minerals to catalyze redox reactions in nature and a bulk low-spin Fe mineral, needs to provide high-spin Fe on surfaces to moderate spin-forbidden transitions. In this work, the spin state of pyrite is investigated using density functional theory (DFT) calculations on cluster and periodic models. The energies of clusters Fe x S 2 x (where x = 4, 8, 16, and 32) were calculated as a function of total spin and different up/down spin configurations. The undercoordinated Fe on surfaces, edges, and corners were found to provide intermediate and high-spin Fe necessary for catalysis. Generally, the lower the crystal field splitting energy (CFSE), Δ, for a particular Fe atom, the higher is the spin density. Pyrite bulk (3D) and surfaces (2D) (+ water to mimic aqueous systems) were examined. The calculated bulk band gap (0.95 eV) is in excellent agreement with previous reports. For the surface, a conducting state is predicted. The calculated CFSE for bulk Fe( II ) in pyrite (~2.2 eV) agrees with previous CFT results; due to surface states, this CFSE decreases to ~1 eV on terraces. This study highlights the importance of accurately describing the spin state of pyrite.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Functional Photoresists for Energy Applications. Final Report

Monolithic ultralow-density porous bulk materials have recently attracted much interest due to many emerging applications in the areas of catalysis, energy storage and conversion, and thermal insulation. They are also important components of high energy density (HED) and inertial confinement fusion (ICF) targets. However, despite tremendous progress that has been made in the synthesis of porous materials, deterministic and independent control over microscopic architecture, density and composition remain key issues, and their integration in high precision devices requires cost and time-intensive mechanical machining that not only reduces reproducibility by generating debris but also limits the complexity of the 3D shapes that can be realized. In this project, we overcame these limitations by developing a universal templating capability that provides deterministic and independent control over density, composition, architecture, and macroscopic sample shape. This was achieved by developing the technology to 1) 3D print ultrahigh resolution, ultra-high precision polymeric micro-lattice templates, 2) coat these templates with the desired materials, and 3) removing the template (Fig. 1a). Atomic layer deposition (ALD) provides the atomic scale coating thickness accuracy required for precisely controlling density. While this templating approach had been demonstrated in prior work, limitations in suitable photoresists, 3D print technologies, print design, and template removal techniques did not allow the fabrication of millimeter-sized high-precision parts with sub-micron resolution. To enable this technology, we developed 1) two-photon polymerization (TPP) print designs that enable the fabrication of millimeter-sized, mechanically robust polymeric templates with sub-micron resolution and 2) a continuum level TPP printing simulation capability for additional print design guidance; 3) atomistic models to study photoresist polymerization kinetics and network topography, 4) refractive index matched polymeric and preceramic TPP photoresists, and 5) functional TPP photoresists including porous voxel structures and self-immolative polymer photoresist chemistries; and 6) damage free template removal techniques that enable the fabrication of defect-free high-precision low-density foam components. We also developed a templating approach for pure carbon microlattices with a unique tube-in-tube ligament morphology. As a test platform, we pursued the fabrication of foam liners that promise to further increase the neutron yield in indirect drive ICF experiments by improving implosion symmetry control and coupling between the laser and the deuterium-tritium fuel. This application requires fabrication and integration of a ultra-high precision, millimeter-sized, thin-walled (200-400 micrometer thick), low-density (10-30 mg/cc), high atomic number (high Z) cylindrical foam tube into the gold hohlraum of an indirect drive ICF target (Fig. 1b). While our hohlraum liner test case will mainly find application in HED and ICF experiments, the underlying science will also directly apply to previously developed nanoparticle and additive manufacturing technologies and will advance those techniques as well.

36 MATERIALS SCIENCE↗

Galileo observations of the motions of ion and electron plasmas in the magnetotail

A series of simultaneous determinations is presented of the 3D bulk flows of ion and electron plasmas in the magnetotail at radial distances near the lunar orbit. In the plasma mantle the ion and electron bulk velocities are identical within measurement accuracy. In the plasma sheet the electron bulk flows, densities, and temperatures are consistent with the results of the previous ISEE-3 survey at these radial distances as given by Zwickl et al. (1984). The present observations show that the electron bulk flows are often dominantly field-aligned and attributable to field-aligned currents, not convective motions within the magnetotail. The E x B convection of the plasmas as determined directly from the ion observation is often significantly slower and/or in a different direction than the bulk motions of either the ion or the electron plasmas. Thus, the ISEE-3 observations of electron bulk flows cannot be reliably used as measures of the E x B convection of plasmas or ion bulk motions at these distances in the plasma sheet.

Frank, L. A.↗

Stability of low-carrier-density topological-insulator Bi{sub 2}Se{sub 3} thin films and effect of capping layers

Although over the past number of years there have been many advances in the materials aspects of topological insulators (TIs), one of the ongoing challenges with these materials is the protection of them against aging. In particular, the recent development of low-carrier-density bulk-insulating Bi{sub 2}Se{sub 3} thin films and their sensitivity to air demands reliable capping layers to stabilize their electronic properties. Here, we study the stability of the low-carrier-density Bi{sub 2}Se{sub 3} thin films in air with and without various capping layers using DC and THz probes. Without any capping layers, the carrier density increases by ∼150% over a week and by ∼280% over 9 months. In situ-deposited Se and ex situ-deposited poly(methyl methacrylate) suppress the aging effect to ∼27% and ∼88%, respectively, over 9 months. The combination of effective capping layers and low-carrier-density TI films will open up new opportunities in topological insulators.

36 MATERIALS SCIENCE↗

Ultra‐Uniform Nanocrystalline Materials via Two‐Step Sintering

Abstract Nanocrystalline materials with superior properties are of great interest. Much is discussed about obtaining nanograins, but little is known about maintaining grain‐size uniformity that is critical for reliability. An especially intriguing question is whether it is possible to achieve a size distribution narrower than what Hillert theoretically predicted for normal grain growth, a possibility suggested—for growth with a higher growth exponent—by the generalized mean‐field theory of Lifshitz, Slyozov, Wagner (LSW), and Hillert but never realized in practice. Following a rationally designed two‐step sintering route, it has been made possible in bulk materials by taking advantage of the large growth exponent in the intermediate sintering stage to form a uniform microstructure despite residual porosity, and freezing the grain growth thereafter while continuing densification to reach full density. The bulk dense Al 2 O 3 ceramic thus obtained has an average grain size of 34 nm and a size distribution much narrower than Hillert's prediction. Bulk Al 2 O 3 with a grain‐size distribution narrower than the particle‐size distribution of starting powders is also demonstrated, as are highly uniform bulk engineering metals (refractory Mo and W‐Re alloy) and complex functional ceramics (BaTiO 3 ‐based alloys with superior dielectric strength and energy capacity).

Dong, Yanhao↗

Iron-rich perovskite in the Earth;s lower mantle

The equations of state of perovskite with (Mg{sub 0.75},Fe{sub 0.25})SiO{sub 3} and MgSiO{sub 3} compositions have been investigated by synchrotron X-ray diffraction up to 130 GPa at 300 K in diamond anvil cells. Here we show that the addition of 25% Fe in MgSiO{sub 3} perovskite increases its density and bulk sound velocity (V{phi}) by 4-6% and 6-7%, respectively, at lower-mantle pressures. Based on concurrent synchrotron X-ray emission and Moessbauer spectroscopic studies of the samples, the increase in V{phi} and density can be explained by the occurrence of the low-spin Fe3+ and the extremely high-quadrupole component of Fe{sup 2+}. Combining these experimental results with thermodynamic modeling, our results indicate that iron-rich perovskite can produce an increase in density and a value of V{phi} that is compatible with seismic observations of reduced shear-wave velocity in regions interpreted as dense, stiff piles in the lower mantle. Therefore, the existence of the Fe-rich perovskite in the lower mantle may help elucidate the cause of the lower-mantle large low-shear-velocity provinces (LLSVPs) where enhanced density and V{phi} are seismically observed to anti-correlate with the reduced shear wave velocity.

58 GEOSCIENCES↗

Physics-informed machine learning exploration of Na storage mechanisms in disordered carbon

Sodium-ion batteries are a cost-effective, sustainable alternative to lithium-ion systems for large-scale energy storage. However, optimizing sodium storage in carbon-based anodes with microstructural complexity and atomic disorder remains a major challenge. The intrinsic inhomogeneity of these materials produces diverse local environments, making it difficult for conventional methods to predict and control ion dynamics. Hard carbon (HC) anodes, composed of ranges of ordered-to-disordered graphitic and amorphous nanodomains, offer tunable ion storage and rate capacity, yet rationale design remains a challenge due to poorly understood correlation between local atomic feature and ion transport mechanism. Here, to address this challenge, we introduce a data-driven framework that integrates validated machine-learned interatomic potentials, large-scale molecular dynamics simulations, and machine learning to elucidate sodium transport mechanisms as a function of carbon and sodium loading densities. By computing per-ion structural descriptors and applying unsupervised learning, we identify distinct diffusion modes governed by microscopic features. Supervised analysis and correlation mapping then establish quantitative links between these transport regimes and processing variables such as bulk carbon density and sodium content. This physics-informed approach establishes quantitative structure–transport relationships and offers actionable design principles for engineering high-performance HC anodes.

Data-driven framework↗

A Coupled Plasma Dynamics and Gas Flow Model for Semiconductor Processing

A continuum modeling approach by self-consistently coupling plasma dynamics and gas flow will be presented for the analysis of high density plasma reactors. Experimental data shows that gas flow distribution affects the etch rate uniformity even at low pressures (6-20 mTorr) and flow rates (20-70 sccm). This study will investigate the effects of gas flow and gas energy on bulk plasma densities and temperatures using a continuum model. The model solves multidimensional equations of mass balance for neutrals and ions, gas momentum, separate energy equations for electrons and neutrals and Maxwell's equations for power coupling. A test case of N2 plasma in a 300mm TCP etch reactor, for which hybrid model and Langmuir probe data are available, is chosen for this analysis. Our preliminary results show that modeling gas flow and energy improves the predictions of electron density and its spatial variation in the reactor when compared with the experimental data. The aim of this study is to identify the operating conditions for the TCP reactor when a self-consistent modeling of gas flow is important.

Bose, Deepak↗

Room temperature persisting surface charge carriers driven by intense terahertz electric fields in a topological insulator Bi 2 Se 3

Topologically protected surface current is highly promising for next-generation low-dissipation and disorder-tolerant quantum electronics and computing. Yet, electric transport from the co-existing bulk state dominates the responses of the Dirac surface state, especially at elevated temperatures relevant to technological applications. Here, we present an approach that convincingly showcases the generation, disentanglement, and precise control of enduring surface charge carriers on a topological insulator, Bi 2 Se 3 , with high bulk conductivity, all achieved at room temperature. By using pump–probe modulation spectroscopy under ultrabroadband driving tunable from 4 meV to 1.55 eV, we show the terahertz (THz) field-induced surface carriers by discovering their initial temporal responses dominant over high density trivial bulk carriers. Strikingly, the response of the induced surface carrier responses persists for more than ~5 ps and is enhanced by reducing pump photon energy. The dynamics and lifetime of the distinct surface response manifest themselves as the enhanced THz pump-induced THz transmission, which directly correlates with the transient negative THz conductivity. Increasing the THz driving field reduces the induced surface carrier lifetime and identifies, particularly, an optimal pump field of E s ~ 224 kV cm -1 for generating the dominant surface response relative to the bulk. This surface carrier dominant regime is suppressed by a joint effect of enhanced surface-bulk scattering and a more rapid saturation of surface excitation compared to the bulk that sets in above E s . The controllability of room temperature topologically surface carriers through pump photon energy offer compelling possibilities for extending this approach to other topological complex materials.

36 MATERIALS SCIENCE↗

Irreversible Multielement Diffusion and the Resulting Compositional and Processing Flexibility in the Synthesis and Densification of Lithium Aluminum Lanthanum Zirconium Oxide

Despite the broad interest in Al-doped lithium lanthanum zirconium oxide (LLZO), the wide range of reported ionic conductivities suggests that the effect of processing parameters on the resulting phase purity and bulk conductivity is not well-understood. Here, in this work, we synthesized six separate series of LLZO with variations in Al concentration, Li excess, Li addition order, Li source, densification method, and mother powder to determine the effect on the composition, phase purity, density, and bulk conductivity. We found that a wider range of compositions (6.08–7.61 mol of Li and 0.06–0.23 mol of Al) than previously reported can result in cubic phase stability and that nearly all elements (Li, Al, Zr, and La) are lost to the MgO crucible during calcination and sintering. The manner in which different elements are lost is affected by the processing parameters. We observed that Al-doped LLZO shows great compositional flexibility in stabilizing the cubic phase, offering an explanation for the range of electrochemical performance metrics reported in the literature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

High-resolution planar electron beam induced current in bulk diodes using high-energy electrons

Understanding the impact of high-energy electron radiation on device characteristics remains critical for the expanding use of semiconductor electronics in space-borne applications and other radiation harsh environments. Here in this paper, we report on in situ measurements of high-energy electron radiation effects on the hole diffusion length in low threading dislocation density homoepitaxial bulk n-GaN Schottky diodes using electron beam induced current (EBIC) in high-voltage scanning electron microscopy mode. Despite the large interaction volume in this system, quantitative EBIC imaging is possible due to the sustained collimation of the incident electron beam. This approach enables direct measurement of electron radiation effects without having to thin the specimen. Using a combination of experimental EBIC measurements and Monte Carlo simulations of electron trajectories, we determine a hole diffusion length of 264 ± 11 nm for n-GaN. Irradiation with 200 kV electron beam with an accumulated dose of 24 × 10 16 electrons cm -2 led to an approximate 35% decrease in the minority carrier diffusion length.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

A shock-induced phase change in iron-silicate garnet.

Hugoniot measurements on iron-silicate garnet demonstrate that above a shock pressure of about 205 kbar transition to a high-pressure phase(s), having an apparent zero-pressure density and bulk modulus of 4.44 g/cu cm and 3.3 Mbar, occurs. Crystal chemical systematics and Debye-Scherrer X-ray patterns of a recovered phase(s), which may be the shock-induced high-pressure form, suggest possible formation of a phase with a density of 4.48/cu cm. Occurrence of such a polymorph of garnet in the mantle would give rise to an increase in density and seismic velocity below 600 km in the earth.

Ahrens, T. J.↗

A Semi-Empirical Density Law for Ternary, Homogeneous PuCl 3 /HCl/H 2 O Solutions

Nuclear material operations pose unique hazards that are not encountered in other chemical, energy, or manufacturing industries. One of these hazards is the potential for a nuclear criticality accident when handling fissile isotopes such as 235 U and 239 Pu. These hazards are particularly high when fissile material is dissolved in solution as the neutron behaviors of the system can change rapidly with the physical and chemical changes accessible in solution. Current estimates of solution density used for criticality safety are outdated and hinder fissile material handling. Developing new estimates for these safety calculations requires experimental characterization and the derivation of empirical density models. We have derived a density law describing PuCl 3 /HCl/H 2 O solutions from experimental data characterizing solution density. Density data was treated using a Pitzer-derived eight-parameter equation, defining density as a function of analyte concentrations, temperature, and interactions between these variables. The model is predictive across the concentration and temperature ranges from which it was derived. The potential effects of varying oxidation states of plutonium, which are easily accessible in aqueous media, on the bulk solution density of the ternary system were also investigated. The resulting Pitzer-derived density law was applied to a nuclear criticality safety model, and the impact of the experimental characterization of solution density relative to previous estimates was demonstrated to be significant and suggest that the current approach to estimating density in nuclear criticality safety calculations may lead to overly conservative controls.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DE-1 observations of polar O(+) stream bulk parameters and comparison with a model of the centrifugally-accelerated polar wind

A survey of bulk parameters of analyzable O(+) outward streams in the mid-altitude (3-4.7 R(sub E) geocentric distance) polar cap magnetosphere is obtained from measurements by the Retarding Ion Mass Spectrometer (RIMS) aboard the Dynamics Explorer-1 (DE-1) spacecraft. There is wide scatter in the obtained densities, but they do display discernible trends: the average O(+) density in these streams decreases from about 60 ions/cc at 3.5 R(sub E) to about 1 ion/cc at 4.6 R(sub E). The streaming velocities are somewhat more defined, and their average increases from about 8 km/s at 3.5 R(sub E) to about 12 km/s at 4.6 R(sub E). The densities and bulk velocities are inversely correlated. We have further compared these observational trends with model profiles for the centrifugally-accelerated polar wind as recently described by Horwitz et al. (1994). The large outflow velocities observed can be understood in part as centrifugally-driven by convection with ionospheric electric field magnitudes of the order 50-70 mV/m, perhaps including plasma expansion effects.

Ho, C. Wing↗

Plasma observations at Venus with Galileo

Plasma measurements were obtained with the Galileo spacecraft during an approximately 3.5-hour interval in the vicinity of Venus on February 10, 1990. Several crossings of the bow shock in the local dawn sector were recorded before the spacecraft passed into the solar wind upstream from this planet. Solar wind densities and bulk speeds were determined from the electron velocity distributions. A magnetic field-aligned distribution of hotter electrons or 'strahl' was also found in the solar wind. Ions streaming into the solar wind from the bow shock were detected. Electron heating at the bow shock, about 20 percent, was notably small, with substantial density increases by factors of 2 to 3 at the day side of the shock that decrease for shock crossings further downstream from the planet. A search for pickup ions from the hot hydrogen and oxygen planetary coronas yielded an upper limit for these densities in the range of 0.001 ion/cu cm, which is consistent with densities expected from current models of neutral gas densities.

Frank, L. A.↗