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At least 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

Kinetic model for quartz and spinel dissolution during melting of high-level-waste glass batch

The dissolution of quartz particles and the growth and dissolution of crystalline phases during the conversion of batch to glass potentially affects both the glass melting process and product quality. Crystals of spinel exiting the cold cap to molten glass below can be troublesome during the vitrification of iron-containing high-level wastes. To estimate the distribution of quartz and spinel fractions within the cold cap, we used kinetic models that relate fractions of these phases to temperature and heating rate. Fitting the model equations to data showed that the heating rate, apart from affecting quartz and spinel behavior directly, also affects them indirectly via concurrent processes, such as the formation and motion of bubbles. Because of these indirect effects, it was necessary to allow one kinetic parameter (the pre-exponential factor) to vary with the heating rate. The resulting kinetic equations are sufficiently simple for the detailed modeling of batch-to-glass conversion as it occurs in glass melters. The estimated fractions and sizes of quartz and spinel particles as they leave the cold cap, determined in this study, will provide the source terms needed for modeling the behavior of these solid particles within the flow of molten glass in the melter.

Batch melting, Cold cap, Quartz, Spinel, Waste gla↗
DOE OSTI2011

Trends in Ln(III) Sorption to Quartz Assessed by Molecular Dynamics Simulations and Laser Induced Flourescence Studies

Molecular dynamics simulations were performed to examine trends in trivalent lanthanide [Ln(III)] sorption to quartz surface SiOH0 and SiO- sites across the 4f period. Complementary laser induced fluorescence studies examined Eu(III) sorption to quartz at varying ionic strength such that the surface sorbed species could be extrapolated at zero ionic strength, the conditions under which the simulations are performed. This allowed for direct comparison of the data, enabling a molecular understanding of the surface sorbed species and the role of the ion surface charge density upon the interfacial reactivity. Thus, this combined theoretical and experimental approach aids in the prediction of the fate of trivalent radioactive contaminants at temporary and permanent nuclear waste storage sites. Potential of mean force molecular dynamics, as well as simulations of pre-sorbed Ln(III) species agrees with the spectroscopic study of Eu(III) sorption, indicating that strongly bound inner-sphere complexes are formed upon sorption to an SiO- site. The coordination shell of the ion contains 6-7 waters of hydration and it is predicted that surface OH groups dissociate from the quartz and bind within the inner coordination shell of Eu(III). Molecular simulations predict less-strongly bound inner2 sphere species in early lanthanides and more strongly bound species in late lanthanides, following trends in the ionic radius of the 4f ions. The participation of surface dissociated OHgroups within the inner coordination shell of the Ln(III) ion is, however, consistent across the series studied. Sorption to a fully protonated quartz surface is not predicted to be favorable by any Ln(III), except perhaps Lu.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2014

Luminescence of silicon dioxide different polymorph modification: Silica glass, α-quartz, stishovite, coesite

Stishovite, coesite, oxygen deficient silica glass as well as irradiated α-quartz, exhibit two luminescence bands: a blue one and an UV one both excitable in the range within optical gap. There are similarities in spectral position and in luminescence decay kinetics among centers in these materials. The interpretation was done on the model of Oxygen Deficient Centers (ODC) [1]. The ODC(II) or twofold coordinated silicon and ODC(I) are distinguished. ODC(I) is object of controversial interpretation. The Si-Si oxygen vacancy [2] and complex defect including latent twofold coordinated silicon [3] are proposed. Remarkably, this luminescence center does not exist in as grown crystalline α-quartz. However, destructive irradiation of α-quartz crystals with fast neutrons, γ rays, or dense electron beams [4–6] creates ODC(I) like defect. In tetrahedron structured coesite the self trapped exciton (STE) luminescence observed with high energetic yield (∼30%) like in α-quartz crystals. STE in coesite coexists with oxygen deficient-like center. In octahedron structured stishovite STE was not found and only ODC exists.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Characterization of silica quartz as raw material in photovoltaic applications

Raw materials are essential for the functioning of modern societies, and access to these raw materials is vital to the world economy. Sustainable development, both globally level, raises important new challenges associated with access and efficient use of raw materials. High purity quartz, is consider as a critical raw material and it is a rare commodity that only forms under geological conditions where a narrow set of chemical and physical parameters is fulfilled. When identified and following special beneficiation techniques, high purity quartz obtains very attractive prices and is applied in high technology sectors that currently are under rapid expansion such as photovoltaic solar cells, silicon metal - oxide wafers in the semiconductor industry and long distance optical fibers that are used in communication networks. Crystalline silicon remains the principal material for photovoltaic technology. Metallurgical silicon is produced industrially by the reduction of silica with carbon in an electric arc furnace at temperatures higher than 2000 °C in the hottest parts, by a reaction that can be written ideally as: SiO{sub 2} + 2C = Si + 2CO. The aim of this study has been to test experimental methods for investigating the various physical and chemical proprieties of Hoggar quartz with different techniques: X Ray Fluorescence, infra-red spectroscopy, Scanning Electron Microscopy, Optic Microscopy, Carbon Analyzer and Vickers Hardness. The results show finally that the quartz has got good result in purity but need enrichment for the photovoltaic application.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Quartz conditioning crystal for X-ray rocking curve topography

A large α-quartz crystal designed to condition the monochromatic beam at beamline 1-BM of the Advanced Photon Source is presented. The purpose of this crystal was to provide a precise match to the Bragg angle of quartz crystals that are commonly used to make analyzers for plasma diagnostics. In order to characterize these analyzers, area detectors need to be positioned at distances from the analyzer at upwards of 1000 mm. As a result of this precise matching, a Bragg-reflected beam from such an analyzer is precisely parallel to the beam incident on the conditioning crystal. This situation alleviates the need to adjust the position of the area detector as the distance between the analyzer and the area detector is varied. That is, there is no need to account for vertical displacement of the diffracted-beam image as a function of this distance. Additionally, verification that the analyzer is set to the correct Bragg reflection is obtained by scanning this distance, because only for a spurious reflection will there be a vertical displacement. This is a very useful check. To commission the conditioning crystal, diffraction from a high-quality flat quartz crystal was mapped using a CCD. Bragg diffraction from the 40$\bar{40}$ reflection at 8.5 keV was studied over an area of 23 × 31 mm. The theoretical Darwin width of the flat sample in this case was 4.7 µrad. An FWHM value near 6 µrad was measured over almost the entire mapped area. These data demonstrate that the resolution function for this four-crystal arrangement is ~4 µrad. Data are also presented for a 0.1 mm-thick α-quartz wafer pressed into a concave form, having a nominal radius of 500 mm and intended for use as an analyzer. Because analyzers are bent crystals, diffraction occurs in narrow bands. When a multiple exposure is made as a function of rocking angle a striped pattern is obtained, which is commonly referred to as a zebra-stripe pattern. A series of zebra stripes from the 30$\bar{33}$ Bragg reflection of the bent wafer over its 25 mm-diameter area were recorded on a CCD. The zebra-stripe pattern was analyzed to show a uniform bending to a radius of 497.0 ± 0.3 mm, in support of the nominal value. An r.m.s. slope error of 7 µrad was also obtained from this analysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Supereruption quartz crystals and the hollow reentrants

Hollow reentrants in quartz phenocrysts from Yellowstone (western United States) caldera’s Lava Creek Tuff are preserved vestiges of bubbles in the supereruption’s pre-eruptive magma reservoir. We characterized the reentrants using a combination of petrographic techniques, synchrotron X-ray microtomography, and cathodoluminescence imagery. One or more reentrants occur in ~20% of quartz, and up to ~90% of those reentrants are hollow. The earliest-erupted parts of the Lava Creek Tuff have the most empty reentrants. The hollow reentrants provide direct, physical evidence for volatile saturation, exsolution, and retention in a magma reservoir. Quartz-melt surface tension permits bubbles to attach to quartz only when bubbles have been able to nucleate and grow in the melt. Prior to eruption, the Lava Creek Tuff existed as a bubbly, volatile-saturated magma reservoir. Finally, the exsolved volatiles increased magma compressibility, helping to prevent the ever-accumulating magma from reaching a critical, eruptive overpressure until it reached a tremendous volume.

58 GEOSCIENCES↗
DOE OSTI2011

Phlogopite and Quartz Lamellae in Diamond-bearing Diopside from Marbles of the Kokchetav Massif Kazakhstan: Exsolution or Replacement Reaction

Exsolution lamellae of pyroxene in garnet (grt), coesite in titanite and omphacite from UHPM terranes are widely accepted as products of decompression. However, interpretation of oriented lamellae of phyllosilicates, framework silicates and oxides as a product of decompression of pyroxene is very often under debate. Results are presented here of FIB-TEM, FEG-EMP and synchrotron-assisted infrared (IR) spectroscopy studies of phlogopite (Phlog) and phlogopite + quartz (Qtz) lamellae in diamond-bearing clinopyroxene (Cpx) from ultra-high pressure (UHP) marble. These techniques allowed collection of three-dimensional information from the grain boundaries of both the single (phlogopite), two-phase lamellae (phlogopite + quartz), and fluid inclusions inside of diamond included in K-rich Cpx and understanding their relationships and mechanisms of formation. The Cpx grains contain in their cores lamellae-I, which are represented by topotactically oriented extremely thin lamellae of phlogopite (that generally are two units cell wide but locally can be seen to be somewhat broader) and microdiamond. The core composition is: (Ca{sub 0.94}K{sub 0.04}Na{sub 0.02})(Al{sub 0.06}Fe{sub 0.08}Mg{sub 0.88})(Si{sub 1.98}Al{sub 0.02})O{sub 6.00}. Fluid inclusions rich in K and Si are recognized in the core of the Cpx, having no visible connections to the lamellae-I. Lamellar-II inclusions consist of micron-size single laths of phlogopite and lens-like quartz or slightly elongated phlogopite + quartz intergrowths; all are situated in the rim zone of the Cpx. The composition of the rim is (Ca{sub 0.95}Fe{sub 0.03}Na{sub 0.02})(Al{sub 0.05}Fe{sub 0.05}Mg{sub 0.90})Si{sub 2}O{sub 6}, and the rim contains more Ca, Mg than the core, with no K there. Such chemical tests support our microstructural observations and conclusion that the phlogopite lamellae-I are exsolved from the K-rich Cpx-precursor during decompression. It is assumed that Cpx-precursor was also enriched in H{sub 2}O, because diamond included in the core of this Cpx contains fluid inclusions. The synchrotron IR spectra of such diamond record the presence of OH{sup -} stretching and H{sub 2}O bending motion regions. Lamellar-II inclusions are interpreted as forming partly because of modification of the lamellae-i in the presence of fluid enriched in K, Fe and Si during deformation of the host diopside; the latter is probably related to the shallower stage of exhumation of the UHP marble. This study emphasizes that in each case to understand the mechanism of lamellar inclusion formation more detailed studies are needed combining both compositional, structural and three-dimensional textural features of lamellar inclusions and their host.

58 GEOSCIENCES↗
DOE OSTI2012

Mineral Dissolution and Secondary Precipitation on Quartz Sand in Simulated Hanford Tank Solutions Affecting Subsurface Porosity

Highly alkaline nuclear waste solutions have been released from underground nuclear waste storage tanks and pipelines into the vadose zone at the U.S. Department of Energy’s Hanford Site in Washington, causing mineral dissolution and re-precipitation upon contact with subsurface sediments. High pH caustic NaNO3 solutions with and without dissolved Al were reacted with quartz sand through flow-through columns stepwise at 45, 51, and 89°C to simulate possible reactions between leaked nuclear waste solution and primary subsurface mineral. Upon reaction, Si was released from the dissolution of quartz sand, and nitrate-cancrinite [Na8Si6Al6O24(NO3)2] precipitated on the quartz surface as a secondary mineral phase. Both steady-state dissolution and precipitation kinetics were quantified, and quartz dissolution apparent activation energy was determined. Mineral alteration through dissolution and precipitation processes results in pore volume and structure changes in the subsurface porous media. In this study, the column porosity increased up to 40.3% in the pure dissolution column when no dissolved Al was present in the leachate, whereas up to a 26.5% porosity decrease was found in columns where both dissolution and precipitation were observed because of the presence of Al in the input solution. The porosity change was also confirmed by calculation using the dissolution and precipitation rates and mineral volume changes.

alkaline nuclear waste solution↗
DOE OSTI2023

E-beam-enhanced solid-state mechanical amorphization of α-quartz: Reduced deformation barrier via localized excess electrons as network modifiers

Under hydrostatic pressure, α-quartz (α-SiO 2 ) undergoes solid-state mechanical amorphization wherein the interpenetration of [SiO 4 ] 2- tetrahedra occurs and the material loses crystallinity. This phase transformation requires a high hydrostatic pressure of 14GPa because the repulsive forces resulting from the ionic nature of the Si–O bonds prevent the severe distortion of the atomic configuration. Herein, we experimentally and computationally demonstrate that e-beam irradiation changes the nature of the interatomic bonds in α-quartz and enhances the solid-state mechanical amorphization at nanoscale. Specifically, during in situ uniaxial compression, a larger permanent deformation occurs in α-quartz submicron pillars compressed during e-beam irradiation than in those without e-beam irradiation. Microstructural analysis reveals that the large permanent deformation under e-beam irradiation originates from the enhanced mechanical amorphization of α-quartz and the subsequent viscoplastic deformation of the amorphized region. Further, atomic-scale simulations suggest that the delocalized excess electrons introduced by e-beam irradiation move to highly distorted atomic configurations and alleviate the repulsive force, thus reducing the barrier to the solid-state mechanical amorphization. In conclusion, these findings deepen our understanding of electron–matter interactions and can be extended to new glass forming and processing technologies at nano- and microscale.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Structural match of heterogeneously nucleated Mn(OH) 2 (s) nanoparticles on quartz under various pH conditions

The early nucleation stage of Mn (hydr)oxide on mineral surfaces is crucial to understand its occurrence and the cycling of nutrients in environmental systems. However, there are only limited studies on the heterogeneous nucleation of Mn(OH) 2 (s) as the initial stage of Mn (hydr)oxide precipitation. Here, we investigated the effect of pH on the initial nucleation of Mn(OH) 2 (s) on quartz. Under various pH conditions of 9.8, 9.9, and 10.1, we analyzed the structural matches between quartz and heterogeneously nucleated Mn(OH) 2 (s). The structural matches were calculated by measuring lateral and vertical dimensions using grazing incidence small angle X-ray scattering (GISAXS) and atomic force microscopy (AFM), respectively. We found that a poorer structural match occurred at a higher pH than at a lower pH. The faster nucleation at a higher pH condition accounted for the observed poorer structural match. By fitting the structural match using classical nucleation theory, we also calculated the interfacial energy between Mn(OH) 2 (s) and water (γ nf = 71 ± 7 mJ/m 2 ). The calculated m values and γ nf provided the variance of interfacial energy between quartz and Mn(OH) 2 (s): γ sn = 262–272 mJ/m 2 . As a result, this study provides new qualitative and quantitative information about heterogeneous nucleation on environmentally an abundant mineral surface, quartz, and it offers important underpinnings for understanding the fate and transport of trace ions in environmental systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Heterogeneous Ni- and Cd-Bearing Ferrihydrite Precipitation and Recrystallization on Quartz under Acidic pH Condition

Ferrihydrite, as one of the most common naturally occurring iron oxides, can sequester toxic metals through co-precipitation. In this study, using grazing-incidence small-angle X-ray scattering, the heterogeneous precipitation of pure, Ni-, and Cd-bearing ferrihydrite on quartz was quantified in 0.1 mM Fe 3+ solutions in the absence and presence of 1 mM Ni 2+ or Cd 2+ (pH 3.8 ± 0.1). Under acidic condition, the limited hydrolysis of metal ions resulted in their small amounts of incorporation in ferrihydrite lattices (<0.1%), several orders of magnitude lower than those reported at neutral and alkaline pH conditions. The presence of Ni 2+ or Cd 2+ did not significantly affect the surface charges of either ferrihydrite pre-nucleation clusters (PNCs) or quartz surfaces. Therefore, with similar electrostatic interactions between PNCs and quartz, similar initial heterogeneous precipitation rates of pure and Ni- and Cd-bearing ferrihydrite on quartz were observed. Later on, continuous heterogeneous nucleation and growth of ferrihydrite nanoparticles resulted in their increased polydispersity, and the size-dependent solubility of ferrihydrite nanoparticles caused the Ostwald ripening process. The presence of Ni and Cd was found to retard the recrystallization of ferrihydrite, probably as a result of their structural incorporation, which could inhibit the dissolution of ferrihydrite. Furthermore, this study provided new kinetic and mechanistic insights for understanding the effects of metal ions on the heterogeneous precipitation and recrystallization processes of ferrihydrite nanoparticles on mineral surfaces, which can better predict the fate and transport of heavy metals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Phase-referenced nonlinear spectroscopy of the α-quartz/water interface

Probing the polarization of water molecules at charged interfaces by second harmonic generation spectroscopy has been heretofore limited to isotropic materials. Here we report non-resonant nonlinear optical measurements at the interface of anisotropic z-cut α-quartz and water under conditions of dynamically changing ionic strength and bulk solution pH. We find that the product of the third-order susceptibility and the interfacial potential, χ (3) × Φ(0), is given by (χ1 (3) –iχ2 (3) ) × Φ(0), and that the interference between this product and the second-order susceptibility of bulk quartz depends on the rotation angle of α-quartz around the z axis. Our experiments show that this newly identified term, iχ (3) × Φ(0), which is out of phase from the surface terms, is of bulk origin. Lastly, the possibility of internally phase referencing the interfacial response for the interfacial orientation analysis of species or materials in contact with α-quartz is discussed along with the implications for conditions of resonance enhancement.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2017

Extension of the Hugoniot and analytical release model of α -quartz to 0.2–3 TPa

In recent years, α-quartz has been used prolifically as an impedance matching standard in shock wave experiments in the multi-Mbar regime (1 Mbar = 100 GPa = 0.1 TPa). This is due to the fact that above ~90–100 GPa along the principal Hugoniot α-quartz becomes reflective, and thus, shock velocities can be measured to high precision using velocity interferometry. The Hugoniot and release of α-quartz have been studied extensively, enabling the development of an analytical release model for use in impedance matching. However, this analytical release model has only been validated over a range of 300–1200 GPa (0.3–1.2 TPa). Furthermore, we extend this analytical model to 200–3000 GPa (0.2–3 TPa) through additional α-quartz Hugoniot and release measurements, as well as first-principles molecular dynamics calculations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Torque Differential Magnetometry Using the qPlus Mode of a Quartz Tuning Fork

A quartz tuning fork is the key component of high-resolution atomic force microscope. Because of its high quality factor, a quartz tuning fork can also be used for high-sensitivity magnetometry. In this work, we develop a highly sensitive torque differential magnetometry using the qPlus mode of a quartz tuning fork. The tuning fork is driven by an ac voltage, and its deflection is measured by the resultant ac current. We observe a sharp resonance of the quartz tuning fork at low temperatures down to 1.6 K. We calibrate our torque differential magnetometry by measuring the angular dependence of the hysteresis loop in single-crystal Fe 0.25 TaS 2 . Furthermore, we demonstrate the high sensitivity of the torque differential magnetometry by measuring the quantum oscillations of a bismuth single crystal. The extracted Fermi-surface cross sections are consistent with those of bismuth crystals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

High-pressure phase transitions of α-quartz under nonhydrostatic dynamic conditions: A reconnaissance study at PETRA III

Hypervelocity collisions of solid bodies occur frequently in the solar system and affect rocks by shock waves and dynamic loading. A range of shock metamorphic effects and high-pressure polymorphs in rock-forming minerals are known from meteorites and terrestrial impact craters. In this paper, we investigate the formation of high-pressure polymorphs of α-quartz under dynamic and nonhydrostatic conditions and compare these disequilibrium states with those predicted by phase diagrams derived from static experiments under equilibrium conditions. We create highly dynamic conditions utilizing a mDAC and study the phase transformations in α-quartz in situ by synchrotron powder X-ray diffraction. Phase transitions of α-quartz are studied at pressures up to 66.1 and different loading rates. At compression rates between 0.14 and 1.96 GPa s -1 , experiments reveal that α-quartz is amorphized and partially converted to stishovite between 20.7 GPa and 28.0 GPa. Therefore, coesite is not formed as would be expected from equilibrium conditions. With the increasing compression rate, a slight increase in the transition pressure occurs. The experiments show that dynamic compression causes an instantaneous formation of structures consisting only of SiO 6 octahedra rather than the rearrangement of the SiO 4 tetrahedra to form a coesite. Although shock compression rates are orders of magnitude faster, a similar mechanism could operate in impact events.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Structural response of α-quartz under plate-impact shock compression

Because of its far-reaching applications in geophysics and materials science, quartz has been one of the most extensively examined materials under dynamic compression. Despite 50 years of active research, questions remain concerning the structure and transformation of SiO 2 under shock compression. Continuum gas-gun studies have established that under shock loading quartz transforms through an assumed mixed-phase region to a dense high-pressure phase. While it has often been assumed that this high-pressure phase corresponds to the stishovite structure observed in static experiments, there have been no crystal structure data confirming this. In this study, we use gas-gun shock compression coupled with in situ synchrotron x-ray diffraction to interrogate the crystal structure of shock-compressed α-quartz up to 65 GPa. Our results reveal that α-quartz undergoes a phase transformation to a disordered metastable phase as opposed to crystalline stishovite or an amorphous structure, challenging long-standing assumptions about the dynamic response of this fundamental material.

58 GEOSCIENCES↗
DOE OSTI2019

High x-ray resolving power utilizing asymmetric diffraction from a quartz transmission crystal measured in the 6 keV to 22 keV energy range

We report a Cauchois-type spectrometer utilizing the (203) lattice planes at an oblique angle of 11.53° to the normal to the surface of a quartz transmission crystal recorded the Kα and Kβ spectral lines of six elements from Fe to Ag in the 6–22 keV energy range from a laboratory x-ray source. After deconvolving the natural lifetime widths and the image plate detector broadening from the observed spectral linewidths, the intrinsic crystal resolving power was determined to be 4000 at the lower energies and decreasing to 1000 at the higher energies. Previously, a Si wafer crystal exhibited twice this resolving power when the (331) planes had been used in asymmetric geometry. The investigation of diffraction with this quartz crystal, with a very similar lattice spacing and therefore spectral coverage, was motivated by the larger integrated reflectivity of quartz due to its well-known quasimosaicity upon elastic bending. The measured spectral linewidths were in good agreement with the widths calculated by accounting for various broadening mechanisms, including source size, crystal thickness, crystal height, crystal rocking curve width, geometrical aberrations, and possible spectrometer configuration errors. This is the first, to the best of our knowledge, demonstration of high resolving power achieved by asymmetric diffraction over a wide energy range (6–22 keV) and with detailed comparisons with theoretical broadenings. Finally, based on these results, Cauchois spectrometers employing asymmetric planes of perfect quartz and silicon crystals can be reliably designed and optimized for high-resolution spectroscopy in the >6 keV energy range.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Quartz Clock Oscillator Design and Analysis

Engineers at Sandia National Laboratories (SNL) have used quartz - based clock oscillators in various missions since the 1980s. As such, the design of these frequency control devices requires a high degree of reliability and producibility. The quartz clock oscillators designed at SNL have evolved over many years and are currently developed in house and fabricated using SNLs internal CMOS foundry. They are designed to operate in harsh environments, including temperature, radiation, shock and vibration. This report documents the methodology behind the design of quartz clock oscillators developed at SNL and includes an overview of quartz resonator technology and usage guidelines and a detailed overview of oscillator circuits.

42 ENGINEERING↗