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At least 1,081 records · Page 60
All sourcesNASA NTRSDOE OSTI
NASA NTRS2014

Expanding the REE Partitioning Database for Lunar Materials

Positive europium anomalies are ubiquitous in the plagioclase-rich rocks of the lunar highlands, and complementary negative Eu anomalies are found in most lunar basalts. This is taken as evidence of a large-scale differentation event, with crystallization of a global-scale lunar magma ocean (LMO) resulting in a plagioclase flotation crust and a mafic lunar interior from which mare basalts were later derived. However, the extent of the Eu anomaly in lunar rocks is variable. Some plagioclase grains in a lunar impact rock (60635) have been reported to display a negative Eu anomaly, or in some cases single grains display both positive and neagtive anomalies. Cathodoluminescence images reveal that some crystals have a negative anomaly in the core and positive at the rim, or vice versa, and the negative anomalies are not associated with crystal overgrowths. Oxygen fugacity is known to affect Eu partitioning into plagioclase, as under low fO2 conditions Eu can be divalent, and has an ionic radius similar to Ca2+ - significant in lunar samples where plagioclase compositions are predominantly anorthitic. However, there are very few experimental studies of rare earth element (REE) partitioning in plagioclase relevant to lunar magmatism, with only two plagioclase DEu measurements from experiments using lunar materials, and little data in low fO2 conditions relevant to the Moon. We report on REE partitioning experiments on lunar compositions. We investigate two lunar basaltic compositions, high-alumina basalt 14072 and impact melt breccia 60635. These samples span a large range of lunar surface bulk compositions. The experiments are carried out at variable fO2 in 1 bar gas mixing furnaces, and REE are analysed by and LA-ICP-MS. Our results not only greatly expand the existing plagioclase DREE database for lunar compositions, but also investigate the significance of fO2 in Eu partitioning, and in the interpretation of Eu anomalies in lunar materials.

Rapp, Jennifer F.↗
DOE OSTI2020

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

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

36 MATERIALS SCIENCE↗
DOE OSTI2016

Facilitated Ion Transport in Smectic Ordered Ionic Liquid Crystals

We investigated a novel ionic mixture of an imidazolium-based room temperature IL containing ethylene oxide functionalized phosphite anion and a lithium salt that self-assembles into a smectic-ordered IL crystal. The two key features in this work are the unique origin of the smectic order of the ionic mixtures and the facilitated ion transport behavior in the smectic ordered IL crystal. In fact, the IL crystals are self-assembled through Coulombic interactions between ion species, not through the hydrophilic-phobic interactions between charged ion heads and hydrophobic long alkyl pendants or the steric interaction between mesogenic moieties. Furthermore, the smectic order in the IL crystal ionogel facilitates exceptional and remarkable ionic transport. Large ionic conductivity, viscoelastic robustness, and additional electrochemical stability of the IL crystal ionogels provide promising opportunities for future electrochemical applications.

Environmental Molecular Sciences Laboratory↗
NASA NTRS2006

Silica and Pyroxene in IVA Irons; Possible Formation of the IVA Magma by Impact Melting and Reduction of L-LL-Chondrite Materials Followed by Crystallization and Cooling

Group IVA is a large magmatic group of iron meteorites. The mean DELTA O-17 (= delta O-17 - 0.52(raised dot) delta O-18) of the silicates is approx. plus or minus 1.2%o, similar to the highest values in L chondrites and the lowest values in LL chondrites; delta O-18 values are also in the L/LL range. This strongly suggests that IVA irons formed by melting L-LL parental material, but the mean Ni content of IVA irons (83 mg/g) is much lower than that of a presumed L-LL parent (approx. 170 mg/g) and the low-Ca pyroxene present in two IVA meteorites is Fs13, much lower than the Fs20-29 values in L and LL chondrites. Thus, formation from L-LL precursors requires extensive addition of metallic Fe, probably produced by reduction of FeS and FeO. Group IVA also has S/Ni, Ga/Ni, and Ge/Ni ratios that are much lower than those in L-LL chondrites or any chondrite group that preserves nebular compositions, implying loss of these volatile elements during asteroidal processing. We suggest that these reduction and loss processes occurred near the surface of the asteroid during impact heating, and resulted partly from reduction by C, and partly from the thermal dissociation of FeS and FeO with loss of O and S. The hot (approx. 1770 K) low-viscosity melt quickly moved through channels in the porous asteroid to form a core. Two members of the IVA group, Sao Joao Nepomuceno (hereafter, SJN) and Steinbach, contain moderate amounts of orthopyroxene and silica, and minor amounts of low-Ca clinopyroxene. Even though SJN formed after approx. 26% crystallization and Steinbach formed after approx. 77% Crystallization of the IVA core, both could have originated within several tens of meters of the core-mantle interface if 99% of the crystallization occurred from the center outwards. Two other members of the group (Gibeon and Bishop Canyon) contain tabular tridymite, which we infer to have initially formed as veins deposited from a cooling SiO-rich vapor. The silicates were clearly introduced into IVA irons after the initial magma crystallized. Because the y-iron crystals in SJN are typically about 5 cm across, an order of magnitude smaller than in IVA irons that do not contain massive silicates, we infer that the metal was in the gamma-iron field when the silicates were injected. The SJN and Steinbach silicate compositions are near the low-Ca-pyroxene/silica eutectic compositions. We suggest that a tectonic event produced a eutectic-like liquid and injected it together with unmelted pyroxene grains into fissures in the solid metal core. Published estimates of IVA metallographic cooling rates range from 20 to 3000 K/Ma, leading to a hypothesized breakup of the core during a major impact followed by scrambling of the core and mantle debris [Haack, H., Scott, E.R.D., Love, S.G., Brearley, A. 1996. Thermal histories of IVA stony-iron and iron meteorites: evidence for asteroid fragmentation and reaccretion. Geochim. Cosmochim. Acta 60, 3103-3113]. This scrambling model is physically implausible and cannot explain the strong correlation of estimated cooling rates with metal composition. Previous workers concluded that the low-Ca clinopyroxene in SJN and Steinbach formed from protopyroxene by quenching at a cooling rate of 10(sup 12) K/Ma, and suggested that this also supported an impact-scrambling model. This implausible spike in cooling rate by a factor of 10(sup 10) can be avoided if the low-Ca clinopyroxene were formed by a late shock event that converted orthopyroxene to clinopyroxene followed by minimal growth in the clinopyroxene field, probably because melt was also produced. We suggest that metallographic cooling-rate estimates (e.g., based on island taenite) giving similar values throughout the metal compositional range are more plausible, and that the IVA parent asteroid can be modeled by monotonic cooling followed by a high-temperature impact event that introduced silicates into the metal and a low-temperature impact event that partially converted thopyroxene into low-Ca clinopyroxene.

Wasson, John T.↗
DOE OSTI2021

Removal of spurious data in Bragg coherent diffraction imaging: an algorithm for automated data preprocessing

Bragg coherent diffraction imaging (BCDI) provides a powerful tool for obtaining high-resolution structural information from nanocrystalline materials. Here a BCDI sample consisting of a large number of randomly oriented nanoscale crystals is considered. Ideally, only one crystal is oriented to produce a Bragg peak on the detector. However, diffraction from other crystals often produces additional signals on the detector. Before the measured diffraction patterns can be processed into structural images, scientists routinely need to manually identify and remove the `alien' intensities from sources other than the intended crystal. With the development of modern high-coherence storage rings, such as the upgraded Advanced Photon Source (APS), the already slow process of manual preprocessing will be untenable for the large volumes of data that will be produced. An automated method of identifying and deleting alien intensities is proposed. This method exploits the fact that BCDI of a perfect crystal produces diffraction data with inversion symmetry around the Bragg peak. This approach uses the machine learning clustering method DBSCAN to distinguish between diffraction from multiple sources, and then calculates cluster size and inversion symmetry to assess whether clusters of intensity belong to desired data or alien signals. This approach can dramatically reduce the amount of time spent manually processing data, allowing BCDI data processing capabilities to keep pace with the technological advances of fourth-generation synchrotron light sources.

36 MATERIALS SCIENCE↗
NASA NTRS1980

The effect of growth rate, diameter and impurity concentration on structure in Czochralski silicon crystal growth

It is demonstrated that maximum growth rates of up to 80% of the theoretical limit can be attained in Czochralski-grown silicon crystals while maintaining single crystal structure. Attaining the other 20% increase is dependent on design changes in the grower, to reduce the temperature gradient in the liquid while increasing the gradient in the solid. The conclusions of Hopkins et al. (1977) on the effect of diameter on the breakdown of structure at fast growth rates are substantiated. Copper was utilized as the test impurity. At large diameters (greater than 7.5 cm), concentrations of greater than 1 ppm copper were attained in the solid (45,000 ppm in the liquid) without breakdown at maximum growth speeds. For smaller diameter crystals, the sensitivity of impurities is much more apparent. For solar cell applications, impurities will limit cell performance before they cause crystal breakdown for fast growth rates of large diameter crystals.

Digges, T. G., Jr.↗
DOE OSTI2012

A co-crystal of polyoxometalates exhibiting single-molecule magnet behavior: the structural origin of a large magnetic anisotropy

A polyoxometalate-based {Mn III 3 Mn IV } single-molecule magnet exhibits a large axial anisotropy (D = -0.86 cm -1 ) resulting from a near-parallel alignment of Jahn–Teller axes. Its rigorous three-fold symmetry (i.e. rhombicity E → 0) and increased intercluster separation via co-crystallization effectively hamper quantum tunnelling of the magnetization.

36 MATERIALS SCIENCE↗
DOE OSTI2012

Recent developments in high-temperature photonic crystals for energy conversion

After decades of intense studies focused on cryogenic and room temperature nanophotonics, scientific interest is furthermore growing in high-temperature nanophotonics aimed at solid-state energy conversion. These latest extensive research efforts are spurred by a renewed interest in high temperature thermal-to-electrical energy conversion schemes including thermophotovoltaics (TPV), solar–thermophotovoltaics, solar–thermal, and solar–thermochemical energy conversion systems. This field is profiting tremendously from the outstanding degree of control over the thermal emission properties that can be achieved with nanoscale photonic materials. The key to obtaining high efficiency in this class of high temperature energy conversion is the spectral and angular matching of the radiation properties of an emitter to those of an absorber. Together with the achievements in the field of high-performance narrow bandgap photovoltaic cells, the ability to tailor the radiation properties of thermal emitters and absorbers using nanophotonics facilitates a route to achieving the impressive efficiencies predicted by theoretical studies. In this review, we will discuss the possibilities of emission tailoring by nanophotonics in the light of high temperature thermal-to-electrical energy conversion applications, and give a brief introduction to the field of TPV. We will demonstrate how a class of large area 2D metallic photonic crystals can be designed and employed to efficiently control and tailor the spectral and angular emission properties, paving the way towards new and highly efficient thermophotovoltaic systems and enabling other energy conversion schemes based on high-performance high-temperature nanoscale photonic materials.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2019

Hierarchically-structured large superelastic deformation in ferroelastic-ferroelectrics

Large superelastic deformation in ferroelastic-ferroelectrics (FMs) is a complex phenomenon involving multiple mechanisms operating simultaneously. Understanding how these mechanisms contribute corporately is critical to apply this useful property to the intrinsically brittle FMs, which can therefore display both excellent functional and mechanical performance. Here, we have directly observed and quantitatively analyzed in situ in a transmission electron microscope the three main mechanisms of twinning domain, phase transformation and mobile point defect contributing to extremely large superelastic deformation in single-crystal BaTiO 3 (5.0% strain) and Pb(Mg 1/3 Nb 2/3 )O 3 -PbTiO 3 (10.1% strain). Finally, our results reveal the hierarchical origin of large recoverable strain in “brittle” FMs.

36 MATERIALS SCIENCE↗
DOE OSTI2016

MgZnO High Voltage Thin Film Transistors on Glass for Inverters in Building Integrated Photovoltaics

Building integrated photovoltaics (BIPV) have attracted considerable interests because of its aesthetically attractive appearance and overall low cost. In BIPV, system integration on a glass substrate like windows is essential to cover a large area of a building with low cost. But, the conventional high voltage devices in inverters have to be built on the specially selected single crystal substrates, limiting its application for large area electronic systems, such as the BIPV. We demonstrate a Magnesium Zinc Oxide (MZO) based high voltage thin film transistor (HVTFT) built on a transparent glass substrate. We designed devices with unique ring-type structures and use modulated Mg doping in the channel - gate dielectric interface, resulting in a blocking voltage of over 600 V. In addition to BIPV, the MZO HVTFT based inverter technology also creates new opportunities for emerging self-powered smart glass.

14 SOLAR ENERGY↗
DOE OSTI2016

Avilamycin and evernimicin induce structural changes in rProteins uL16 and CTC that enhance the inhibition of A-site tRNA binding

Two structurally unique ribosomal antibiotics belonging to the orthosomycin family, avilamycin and evernimicin, possess activity against Enterococci, Staphylococci, and Streptococci, and other Gram-positive bacteria. Here, we describe the high-resolution crystal structures of the eubacterial large ribosomal subunit in complex with them. Their extended binding sites span the A-tRNA entrance corridor, thus inhibiting protein biosynthesis by blocking the binding site of the A-tRNA elbow, a mechanism not shared with other known antibiotics. Along with using the ribosomal components that bind and discriminate the A-tRNA—namely, ribosomal RNA (rRNA) helices H89, H91, and ribosomal proteins (rProtein) uL16—these structures revealed novel interactions with domain 2 of the CTC protein, a feature typical to various Gram-positive bacteria. Furthermore, analysis of these structures explained how single nucleotide mutations and methylations in helices H89 and H91 confer resistance to orthosomycins and revealed the sequence variations in 23S rRNA nucleotides alongside the difference in the lengths of the eukaryotic and prokaryotic α1 helix of protein uL16 that play a key role in the selectivity of those drugs. Here, the accurate interpretation of the crystal structures that could be performed beyond that recently reported in cryo-EM models provide structural insights that may be useful for the design of novel pathogen-specific antibiotics, and for improving the potency of orthosomycins. Because both drugs are extensively metabolized in vivo, their environmental toxicity is very low, thus placing them at the frontline of drugs with reduced ecological hazards.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2017

Competing spin density wave, collinear, and helical magnetism in Fe 1 + x Te

The Fe 1+x Te phase diagram consists of two distinct magnetic structures with collinear order present at low interstitial iron concentrations and a helical phase at large values of x with these phases separated by a Lifshitz point. In this paper, we use unpolarized single-crystal diffraction to confirm the helical phase for large interstitial iron concentrations and polarized single-crystal diffraction to demonstrate the collinear order for the iron-deficient side of the Fe 1+x Te phase diagram. Polarized neutron inelastic scattering shows that the fluctuations associated with this collinear order are predominately transverse at low-energy transfers, consistent with a localized magnetic moment picture. We then apply neutron inelastic scattering and polarization analysis to investigate the dynamics and structure near the boundary between collinear and helical orders in the Fe 1+x Te phase diagram. We first show that the phase separating collinear and helical orders is characterized by a spin density wave with a single propagation wave vector of (~0.45, 0, 0.5). We do not observe harmonics or the presence of a charge density wave. The magnetic fluctuations associated with this wave vector are different from the collinear phase, being strongly longitudinal in nature and correlated anisotropically in the (H,K) plane. The excitations preserve the C 4 symmetry of the lattice but display different widths in momentum along the two tetragonal directions at low-energy transfers. Finally, while the low-energy excitations and minimal magnetic phase diagram can be understood in terms of localized interactions, we suggest that the presence of the density wave phase implies the importance of electronic and orbital properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

The closo-Si{sub 12}C{sub 12} molecule from cluster to crystal: A theoretical prediction

The structure of closo-Si{sub 12}C{sub 12} is unique among stable Si{sub n}C{sub m} isomers (n, m > 4) because of its high symmetry, π–π stacking of C{sub 6} rings and unsaturated silicon atoms at symmetrical peripheral positions. Dimerization potential surfaces reveal various dimerization reactions that form between two closo-Si{sub 12}C{sub 12} molecules through Si–Si bonds at unsaturated Si atoms. As a result the closo-Si{sub 12}C{sub 12} molecule is capable of polymerization to form stable 1D polymer chains, 2D crystal layers, and 3D crystals. 2D crystal structures formed by side-side polymerization satisfy eight Si valences on each monomer without large distortion of the monomer structure. 3D crystals are formed by stacking 2D structures in the Z direction, preserving registry of C{sub 6} rings in monomer moiety.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Controlled Vapor Phase Growth of Single Crystalline, Two-Dimensional GaSe Crystals with High Photoresponse

Abstract Compared with their bulk counterparts, atomically thin two-dimensional (2D) crystals exhibit new physical properties, and have the potential to enable next-generation electronic and optoelectronic devices. However, controlled synthesis of large uniform monolayer and multi-layer 2D crystals is still challenging. Here, we report the controlled synthesis of 2D GaSe crystals on SiO2/Si substrates using a vapor phase deposition method. For the first time, uniform, large (up to ~60 m in lateral size), single-crystalline, triangular monolayer GaSe crystals were obtained and their atomic resolution structure were characterized. The size, density, shape, thickness, and uniformity of the 2D GaSe crystals were shown to be controllable by growth duration, growth region, growth temperature, and argon carrier gas flow rate. The theoretical modeling of the electronic structure and Raman spectroscopy demonstrate a direct-to-indirect bandgap transition and progressive confinement-induced bandgap shifts for 2D GaSe crystals. The 2D GaSe crystals show p-type semiconductor characteristics and high photoresponsivity (~1.7 A/W under white light illumination) comparable to exfoliated GaSe nanosheets. These 2D GaSe crystals are potentially useful for next-generation electronic and optoelectronic devices such as photodetectors and field-effect transistors.

Li, Xufan↗
DOE OSTI2012

High energy resolution five-crystal spectrometer for high quality fluorescence and absorption measurements on an x-ray absorption spectroscopy beamline

Fluorescence detection is classically achieved with a solid state detector (SSD) on x-ray absorption spectroscopy (XAS) beamlines. This kind of detection however presents some limitations related to the limited energy resolution and saturation. Crystal analyzer spectrometers (CAS) based on a Johann-type geometry have been developed to overcome these limitations. We have tested and installed such a system on the BM30B/CRG-FAME XAS beamline at the ESRF dedicated to the structural investigation of very dilute systems in environmental, material and biological sciences. The spectrometer has been designed to be a mobile device for easy integration in multi-purpose hard x-ray synchrotron beamlines or even with a laboratory x-ray source. The CAS allows to collect x-ray photons from a large solid angle with five spherically bent crystals. It will cover a large energy range allowing to probe fluorescence lines characteristic of all the elements from Ca (Z = 20) to U (Z = 92). It provides an energy resolution of 1-2 eV. XAS spectroscopy is the main application of this device even if other spectroscopic techniques (RIXS, XES, XRS, etc.) can be also achieved with it. The performances of the CAS are illustrated by two experiments that are difficult or impossible to perform with SSD and the complementarity of the CAS vs SSD detectors is discussed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
NASA NTRS1991

Results of the TTF-TCNQ- and the calcium carbonate-crystallization on the Long Duration Exposure Facility

Experiment AO139A on the Long Duration Exposure Facility (LDEF) carried four large containers into orbit for five years with crystal growth solutions for lead sulfide, calcium carbonate, and tetra thiafulvalene- tetra cyanoquino methane (TTF-TCNQ). The LDEF was in excellent condition after the long orbital stay, and although the temperature data was lost, the experiment program had been working since the valves in all containers were opened. All four experiments produced crystals; however, they were of varying quality. The calcium carbonate crystals had the best appearance. The TTF-TCNQ crystals were packed together near the valve openings of the container. When taken apart, the single crystals showed some unusual morphological properties. X-ray investigations as well as conductivity measurements on the long duration space grown TTF-TCNQ crystals are presented, and pictures of the calcium carbonate are shown. Comparisons are made with previous space solution growth experiments on the European Spacelab Mission and the Apollo-Soyuz Test Project.

Nielsen, Kjeld Flemming↗
DOE OSTI2014

Insights into the crystal chemistry of Earth materials rendered by electron density distributions: Pauling's rules revisited

Pauling's first two rules are examined in terms of the accumulation of the electron density between bonded pairs of atoms for a relatively large number of oxide and silicate crystals and siloxane molecules. The distribution of the electron density shows that the radius of the oxygen atom is not fixed, but that it actually decreases systematically from ~1.40 Å to ~ 0.65 Å as the polarizing power and the electronegativity of the bonded metal atoms increase and the distribution of the O atom is progressively polarized and contracted along the bond vectors by the impact of the bonded interactions. The contractions result in an aspherical oxygen atom that displays as many different bonded “radii” as it has bonded interactions. The bonded radii for the metal atoms match the Shannon and Prewitt ionic radii for the more electropositive atoms like potassium and sodium, but they are systematically larger for the more electronegative atoms like aluminum, silicon and phosphorous. Pauling's first rule is based on the assumption that the radius of the oxide anion is fixed and that the radii of the cations are such that radius sum of the spherical oxide anion and a cation necessarily equals the separation between the cation-anion bonded pair with the coordination number of the cation being determined by the ratio of the radii of the cation and anion. In the case of the bonded radii, the sum of the bonded radii for the metal atoms and the oxide anion necessarily equals the bond lengths by virtue of the way that the bonded radii were determined in the partitioning of the electron density along the bond path into metal and O atom parts. But, the radius ratio for the O and M atoms is an unsatisfactory rule for determining the coordination number of the metal atom inasmuch as a bonded O atom is not, in general, spherical, and its size varies substantially along its bonded directions. But by counting the number of bond paths that radiate from a bonded atom, the coordination number of the atom is determined uniquely independent of the asphericity and sizes of the atom. A power law connection established between the bond lengths and bond strengths for crystals and molecules is mirrored by a comparable power law connection between bond length and the accumulation of the electron density between bonded pairs of atoms, a connection that is consistent with Pauling's electroneutrality postulate that the charges of the atoms in an oxide are negligibly small. The connection indicates that a one-to-one correspondence exists between the accumulation between a pair of bonded atoms and the Pauling bond strength for M-O bonded interaction for all atoms of the periodic table. The connection provides a common basis for understanding the success of the manifold applications that have been made with the bond valence theory model together with the modeling of crystal structures, chemical zoning, leaching and cation transport in batteries and the like. We believe that the wide spread applications of the model in mineralogy and material science owes much of its success to the direct connection between bond strength and the quantum mechanical observable, the electron density distribution. Comparable power law expressions established for the bonded interactions for both crystals and molecules support Pauling's assertion that his second rule has significance for molecules as well as for crystals. A simple expression is found that provides a one to one connection between the accumulation of the electron density between bonded M and O atoms and the Pauling bond strength for all M atoms of the periodic table with ~ 95 % of the variation of the bond strength being explained in terms of a linear dependence on the accumulated electron density. Compelling evidence is presented that supports the argument that the Si-O bonded interactions for tiny siloxane molecules and silicate crystals are chemically equivalent.

Environmental Molecular Sciences Laboratory↗