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High Energy Density Physics of Novel Inertial Fusion Energy Amorphous Ablator Materials
Final Report
Free suspension processing of oxides to form amorphous oxide materials, appendix B
The processing of yttria, zirconia, and alumina under weightless conditions is discussed. The process consists of levitation or position control, heating and melting, superheating, and supercooling. The use of arc imaging furnaces, lasers, induction heating, microwave, and electron beam methods are analyzed to show the advantages and disadvantages of each.
Solid-state growth of Si to produce planar surfaces
Paralleling the sophisticated control of Si and GaAs growth from fluid media, we demonstrate control of Si growth using a solid growth medium. Faceted dissolution pits were first produced in a Si substrate using standard photolithographic techniques and Al metallization. Si was then evaporated onto the cold structure, depositing as amorphous material. Upon heating, the amorphous Si migrated through the solid Al and grew rapidly in the faceted pits, typically refilling them flush with the surrounding substrate. Evidence that the rapid growth occurs only while the amorphous Si is dissolving into the Al is presented.
Ionization induced damage in crystalline silicon
Close examination of the interaction of the energetic knock-on atoms with the local lattice environment reveals a damage mechanism which does satisfy the experimental data on proton irradiation of silicon. A proton-atom interaction with high energy transfer is considered where the proton path is delineated by a trail of ionization, and the silicon ion path is characterized by much heavier ionization terminating in a dense displacement cluster. At collision, many of the silicon electrons are stripped off, and the resulting energetic ion subsequently loses energy rapidly by Coulomb interaction with bound electrons. The rate of energy loss depends on the charge state and velocity of the knock-on ion. For ion energies in excess of 1 MeV, the intensity of ionization is sufficient to permit lattice atoms, stripped of their binding electrons, to reorient randomly before having an opportunity to recombine with electrons and re-establish the lattice. The path of a knock-on ion thus becomes a thin cylinder of amorphous material within the crystal. Amorphous silicon has a Fermi level closer to mid-band than does single crystal silicon, and a strong field therefore, results around this damaged region. The field produces a large depletion region, representing a very large capture cross section for minority carriers.
Preparation of amorphous ferromagnetic materials through containerless solidification
The work reported herein consists of: (1) the ground based experiments; (2) the analysis of the ground based specimens; (3) the flight experiment; (4) failure to melt analysis; and (5) recommendations and conclusions. The ground based experimental work yielded new results in terms of understanding the viscoelastic properties of ferromagnetic metallic glasses and the variation of viscosity through the glass transition temperature from metallic glass to crystalline solid. This last result was of importance in predicting what glass can be produced at lower quench rates.
Constraining the Texture and Composition of Pore-Filling Cements at Gale Crater, Mars
The Mars Science Laboratory (MSL) rover Curiosity has encountered a wide variety of sedimentary rocks deposited in fluvio-lacuestrine sequences at the base of Gale Crater. The presence of sedimentary rocks requires that initial sediments underwent diagenesis and were lithified. Lithification involves sediment compaction, cementation, and re-crystallization (or authigenic) processes. Analysis of the texture and composition of the cement can reveal the environmental conditions when the cements were deposited, enabling better understanding of early environments present within Gale Crater. The first step in lithification is sediment compaction. The Gale crater sediments do not show evidence for extensive compaction prior to cementation; the Sheepbed mudstone in Yellowknife Bay (YKB) has preserved void spaces ("hollow nodules"), indicating that sediments were cemented around the hollow prior to compaction, and conglomerates show imbrication, indicating minimal grain reorganization prior to lithification. Furthermore, assuming the maximum burial depth of these sediments is equivalent to the depth of Gale Crater, the sediments were never under more than 1 kb of pressure, and assuming a 15 C/km thermal gradient in the late Noachian, the maximum temperature of diagenesis would have been approximately 75 C. This is comparable to shallow burial diagenetic conditions on Earth. The cementation and recrystallization components of lithification are closely intertwined. Cementation describes the precipitation of minerals between grains from pore fluids, and recrystallization (or authigenesis) is when the original sedimentary mineral grains are altered into secondary minerals. The presence of authigenic smectites and magnetite in the YKB formation suggests that some recrystallization has taken place. The relatively high percentage of XRD-amorphous material (25-40%) detected by CheMin suggests that this recrystallization may be limited in scope, and therefore may not contribute significantly to the cementing material. However, relatively persistent amorphous components could exist in the Martian environment (e.g. amorphous MgSO4), so recrystallization, including loss of crystallinity, cannot yet be excluded as a method of cementation. In order to describe the rock cementation, both the rock textures and their composition must be considered. Here, we attempt to summarize the current understanding of the textural and compositional aspects of the cement across the rocks analyzed by Curiosity to this point.
Investigation of superconducting interactions and amorphous semiconductors
Research papers on superconducting interactions and properties and on amorphous materials are presented. The search for new superconductors with improved properties was largely concentrated on the study of properties of thin films. An experimental investigation of interaction mechanisms revealed no new superconductivity mechanism. The properties of high transition temperature, type 2 materials prepared in thin film form were studied. A pulsed field solenoid capable of providing fields in excess of 300 k0e was developed. Preliminary X-ray measurements were made of V3Si to determine the behavior of cell constant deformation versus pressure up to 98 kilobars. The electrical properties of amorphous semiconducting materials and bulk and thin film devices, and of amorphous magnetic materials were investigated for developing radiation hard, inexpensive switches and memory elements.
Exploring Structural Anisotropy in Amorphous Tb-Co via Changes in Medium-Range Ordering
Amorphous thin films grown by magnetron co-sputtering exhibit changes in atomic structure with varying growth and annealing temperatures. Structural variations influence the bulk properties of the films. Scanning nanodiffraction performed in a transmission electron microscope (TEM) is applied to amorphous Tb 17 Co 83 (a-Tb-Co) films deposited over a range of temperatures to measure relative changes in medium-range ordering (MRO). These measurements reveal an increase in MRO with higher growth temperatures and a decrease in MRO with higher annealing temperatures. The trend in MRO indicates a relationship between the growth conditions and local atomic ordering. By tilting select films, the TEM measures variations in the local atomic structure as a function of orientation within the films. The findings support claims that preferential ordering along the growth direction results from temperature-mediated adatom configurations during deposition, and that oriented MRO correlates with increased structural anisotropy, explaining the strong growth-induced perpendicular magnetic anisotropy found in rare earth–transition metal films. Beyond magnetic films, we propose the tilted FEM workflow as a method of extracting anisotropic structural information in a variety of amorphous materials with directionally dependent bulk properties, such as films with inherent bonding asymmetry grown by physical vapor deposition.
Materials research at Stanford University
Research activity related to the science of materials is described. The following areas are included: elastic and thermal properties of composite materials, acoustic waves and devices, amorphous materials, crystal structure, synthesis of metal-metal bonds, interactions of solids with solutions, electrochemistry, fatigue damage, superconductivity and molecular physics and phase transition kinetics.
Bioinspired mineralizing microenvironments generated by liquid-liquid phase coexistence
Biominerals such as bones, teeth and shells exhibit improved mechanical properties and intricate morphologies not seen in nonbiologically-produced minerals of ostensibly the same composition. These remarkable properties of biogenic minerals are thought to arise due to precise local control over the mineral deposition process, including organic and inorganic inclusions. Understanding how Biology controls the local reaction environment during formation of these materials to control their composition, structure, and properties is a grand challenge that promises to enable new routes to high-performance materials. This project developed multi-compartment bioinspired microreactors as artificial mineralizing vesicles, and used them to understand and control formation of inorganic/organic composite solid materials. A major emphasis was on developing all-aqueous emulsions in which each droplet was a structured microreactor with two or more adjacent phases. This approach provided local control over reaction environment including availability of inclusions such as polypeptides and metal ions, while being sufficiently simple to produce large populations of essentially identical multiphase reactor droplets simultaneously within a batch. Organic/inorganic composite materials could be produced with very high organic content that stabilized the inorganic portions as amorphous materials (e.g., amorphous calcium carbonate) by preventing the typical conversion to more thermodynamically crystalline forms (e.g., calcite). These stabilized amorphous composites could be stored indefinitely and converted to crystalline forms later by removal of the organic inclusions via, for example, heating. Compositional gradients in the organic and inorganic components were embedded during synthesis due to the evolution of the reaction microenvironment, and despite the complexity of this process it occurred similarly across the population of reactive droplets and was hence encoded into the population of resulting composite particles. The approach developed here allows pre-structuring of reactive microenvironments to control the spatiotemporal reaction environment, which is an important step towards rational design and on-demand production of complex functional materials with desired composition, optical properties, and mechanical response.
Revealing the structure and electronic characteristics of Te-rich threshold switching materials for high-density integration
Ovonic threshold switching (OTS) selectors play an important role in the integration of advanced three-dimensional memory. Selectors based on tellurium (Te)-containing materials exhibit significant promise due to their low threshold voltages and superior consistency. Here we have theoretically studied the structure and electronic properties of a typical OTS material, amorphous GeTe 6 , to explore the switching mechanisms using ab initio molecular dynamics simulations. The results indicate that Ge atoms tend to bond with Te atoms, forming stable chemical bonds. The Te-centered clusters are predominantly in the form of distorted octahedrons, while the Ge-centered clusters are in the form of both octahedrons and tetrahedrons. Notably, the proportion of tetrahedrons within the 4-coordinated Ge-centered clusters reaches an impressive 66.9%. These tetrahedrons are randomly dispersed throughout the simulated cell, leading to a stable amorphous configuration. The mid-gap state observed in the mobility bandgap originates from the atomic chain composed of both over-coordinated Ge and Te atoms. It is the inherent stability of the chemical environment within amorphous GeTe 6 that enables it to maintain its amorphous phase under a repeated threshold voltage, a characteristic that distinguishes it from non-OTS materials, such as amorphous tellurium. Furthermore, our findings provide an in-depth understanding of the structure and electronic characteristics of amorphous GeTe 6 , which can promote the design and application of the Te-rich threshold switching materials.
The Chemistry and Mineralogy of Mars Soils: A Tour of Landed Mission Results from the Last 45 years
Eight landed missions demonstrated that martian soils (defined as loose, unconsolidated surface material) consist of basaltic mineralogy, iron (hydr)oxides, amorphous material, sulfate, chloride, (per)chlorate, nitrate, carbonate, and possible organic C. The Viking Lander 1 and 2 (1976), Mars Pathfinder (1997), and Mars Exploration Rover (MER-A,B) (2004) missions determined that martian soil was similar at all landing sites by having mafic chemistry, high S (~ 7 wt.% SO3) and Cl (0.7 wt.%), and spectral detections of poorly crystalline and crystalline Fe-(hydr)oxide phases. The MER Mössbauer spectrometers detected Fe-bearing olivine and pyroxene along with magnetite, nano-phase Fe-oxides (npOx), hematite, and ferric sulfate. The 2008 Phoenix Lander instrumentation measured a soil pH of 7.7 and detected ~0.6 wt.% perchlorate, 3-5 wt.% Ca-rich carbonate and carbon (500 gC/g) consistent with oxidized organics and Fe-rich carbonate. The 2012 Mars Science Laboratory (MSL) rover (Gale Crater) through X-ray diffraction detected plagioclase feldspar, pyroxene, magnetite, hematite, anhydrite, and quartz, with the balance being composed of Si/Fe-containing amorphous (30 to 40 wt.%) material. MSL evolved gas analysis detected (per)chlorate (0.4 wt.% ClO4), nitrate (0.23 wt.%), along with minor Fe/Mg sulfate and oxidized organic C (~2000 gC/g). Limited pedogenesis may have occurred at the 2018 InSight landing site and in one Gusev Crater soil (MER-B) which have 3 to 10 cm-thick duricrust horizons consistent with atmospheric water vapor interactions with soil salts. Martian soil primary mineralogy was derived mostly from local rock (volcanic, sedimentary) that is largely basaltic planet wide. Secondary minerals [e.g., sulfate, chloride, perchlorate, nitrate, carbonate, Fe-(hydr)oxides] in martian soils formed from oxidative aqueous alteration processes and were likely derived from a combination of local sedimentary rock sources and the global bright dust. The Mars 2020 mission will collect soil for Earth return to enable a thorough assessment of the nature and origin of martian soil.
K–Co–Mo–S x chalcogel: high-capacity removal of Pb 2+ and Ag + and the underlying mechanisms
Chalcogenide-based aerogels, known as chalcogels, represent a novel class of nanoparticle-based porous amorphous materials characterized by high surface polarizability and Lewis base properties, exhibiting promising applications in clean energy and separation science. This work presents a K–Co–Mo–S x (KCMS) chalcogel as a highly efficient sorbent for heavy metal ions and details its sorption mechanisms. Its incoherent structure comprises Mo 2 V (S 2 ) 6 and Mo 3 IV S(S 6 ) 2 anion-like clusters with four- and six-coordinated Co–S polyhedra, forming a Co–Mo–S covalent network that hosts K + ions through electrostatic attraction. The interactions of KCMS with heavy metal ions, particularly Pb 2+ and Ag + , reveal that KCMS is exceptionally effective in removing these ions from ppm concentrations down to trace levels (≤5 ppb). KCMS rapidly removes Ag + (≈81.7%) and Pb 2+ (≈99.5%) within five minutes, achieving >99.9% removal within an hour, with a distribution constant K d ≥10 8 mL g -1 . KCMS exhibits an impressive removal capacity of 1378 mg g -1 for Ag + and 1146 mg g -1 for Pb 2+ , establishing it as one of the most effective materials known to date for heavy metal removal. This material is also effective for the removal of Ag + and Pb 2+ along with Hg 2+ , Ni 2+ , Cu 2+ , and Cd 2+ from various water sources even in the presence of highly concentrated and chemically diverse cations, anions, and organic species. Analysis of the post-interacted KCMS by synchrotron X-ray pair distribution function (PDF), X-ray photoelectron spectroscopy (XPS) and energy dispersive X-ray spectroscopy (EDS) revealed that the sorption of Pb 2+ , Ag + , and Hg 2+ mainly occurs by the exchange of K + and Co 2+ . Despite being amorphous, this material exhibits unprecedented ion-exchange mechanisms both for the ionically and covalently bound K + and Co 2+ , respectively. In conclusion, this discovery advances our knowledge of amorphous gels and guides material synthesis principles for the highly selective and efficient removal of heavy metal ions from water.
Three-dimensional atomic packing in amorphous solids with liquid-like structure
Liquids and solids are two fundamental states of matter. However, our understanding of their three-dimensional atomic structure is mostly based on physical models. Here we use atomic electron tomography to experimentally determine the three-dimensional atomic positions of monatomic amorphous solids, namely a Ta thin film and two Pd nanoparticles. We observe that pentagonal bipyramids are the most abundant atomic motifs in these amorphous materials. Instead of forming icosahedra, the majority of pentagonal bipyramids arrange into pentagonal bipyramid networks with medium-range order. Molecular dynamics simulations further reveal that pentagonal bipyramid networks are prevalent in monatomic metallic liquids, which rapidly grow in size and form more icosahedra during the quench from the liquid to the glass state. Furthermore, these results expand our understanding of the atomic structures of amorphous solids and will encourage future studies on amorphous–crystalline phase and glass transitions in non-crystalline materials with three-dimensional atomic resolution.
Cell for measurement of basic electrical properties of amorphous and polycrystalline materials under pressure
Measuring instrument for amorphous and polycrystalline materials resistivity and Seebeck coefficient as function of temperature and pressure
Effects of elevated-temperature deposition on the atomic structure of amorphous Ta 2 O 5 films
Brownian thermal noise as a result of mechanical loss in optical coatings will become the dominant source of noise at the most sensitive frequencies of ground-based gravitational-wave detectors. Experiments found, however, that a candidate material, amorphous Ta 2 O 5 , is unable to form an ultrastable glass and, consequently, to yield a film with significantly reduced mechanical loss through elevated-temperature deposition alone. X-ray scattering PDF measurements are carried out on films deposited and subsequently annealed at various temperatures. Inverse atomic modeling is used to analyze the short and medium range features in the atomic structure of these films. Furthermore, in silico deposition simulations of Ta 2 O 5 are carried out at various substrate temperatures and an atomic level analysis of the growth at high temperatures is presented. It is observed that upon elevated-temperature deposition, short range features remain identical, whereas medium range order increases. After annealing, however, both the short and medium range orders of films deposited at different substrate temperatures are nearly identical. A discussion on the surface diffusion and glass transition temperatures indicates that future pursuits of ultrastable low-mechanical-loss films through elevated temperature deposition should focus on materials with a high surface mobility, and/or lower glass transition temperatures in the range of achievable deposition temperatures.
Formation and energetics of amorphous rare earth (RE) carbonates in the RE 2 O 3 –CO 2 –H 2 O system
Amorphous materials are of interest in the genesis of crystalline solids. They are often the first to precipitate from supersaturated solutions and are in the nanometer size range, transforming into a nanocrystalline metastable phase, and then to thermodynamically stable phases. One must seek knowledge of the composition, structure, thermodynamics, kinetics, and reaction pathways that relate the amorphous and crystalline phases. The subject of this study is the amorphous phases in the system RE 2 O 3 -CO 2 –H 2 O (RE- La, Nd, Dy,Yb). They were synthesized via direct precipitation and urea hydrolysis, and characterized by powder XRD, DTA with mass spectrometric analysis of the evolved gases. Phases have the non-stoichiometric composition RE 2 O 3 ·xCO 2 ·yH 2 O (1 < x < 3, 3 < y <7), which is different from that of crystalline simple carbonates and hydroxycarbonates. Thus we consider them to be amorphous precursors, rather than amorphous carbonates. High temperature oxide melt solution calorimetry in molten sodium molybdate solvent was used to derive their enthalpies of formation from oxides and elements. Increase of energetic stability per mole of RE 2 O 3 compounds occurs in the order: RE 2 O 3 → 2RE(OH)3→ 2REO(OH) → RE 2 O 2 CO 3 → Amorphous precursor → 2(REOHCO 3 ) → RE 2 (CO 3 ) 3 ·yH 2 O. We calculated the enthalpies of possible transformations of amorphous precursors to crystalline phases and conclude that thermodynamics determines the dependence of the crystallizing products on the temperature and partial pressure of CO 2 and H 2 O. Amorphous precursors are clearly intermediate in the synthesis, and ternary phases containing both H 2 O and CO 2 compete with each other in terms of thermodynamic stability. The energy landscape obtained here will allow one to directly synthesize specific products and control their functionality.