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NASA NTRS1973

Debye-Scherrer investigations of experimentally shocked silicates.

Small ballistic ranges were used to perform controlled laboratory shock experiments on 12 selected silicates. Debye-Scherrer investigations of shocked materials revealed a gradual lattice breakdown of crystalline matter under shock. Individual mineral species behave selectively. Sheet silicates break down very easily, followed by tecto-silicates. Chain-, ino- and ortho-silicates are of considerably higher shock resistance. Depending on the mineral species, the first sign of shock damage is evidenced in the long range order at 20-70 kb. At intermediate pressures (100-200 kb) the long range order is essentially destroyed with the short range order heavily disturbed. At pressures exceeding 300 kb tecto-silicates are completely collapsed.

Hoerz, F.↗
NASA NTRS1983

Experimental investigation of the partitioning of phosphorus between metal and silicate phases - Implications for the earth, moon and eucrite parent body

An experimental study is reported of the partitioning of Phosphorus between solid metal and basaltic silicate liquid as a function of temperature and oxygen fugacity and of the implications for the earth, moon and eucrite parent body (EPB). The relationship established between the partition coefficient and the fugacity is given at 1190 C by log D(P) = -1.12 log fO2 - 15.95 and by log D(P) = -1.53 log fO2 17.73 at 1300 C. The partition coefficient D(P) was determined, and it is found to be consistent with a valence state of 5 for P in the molten silicate. Using the determined coefficient the low P/La ratios of the earth, moon, and eucrites relative to C1 chondrites can be explained. The lowering of the P/La ratio in the eucrites relative to Cl chondrite by a factor of 40 can be explained by partitioning P into 20-25 wt% sulfur-bearing metallic liquid corresponding to 5-25% of the total metal plus silicate system. The low P/La and W/La ratios in the moon may be explained by the partitioning of P and W into metal during formation of a small core by separation of liquid metal from silicate at low degrees of partial melting of the silicates. These observations are consistent with independent formation of the moon and the earth.

Newsom, H. E.↗
NASA NTRS1989

The identification of crystalline olivine in cometary silicates

An intermediate-resolution spectrum of the 8-13 micron region in comet Halley is obtained which shows a prominent silicate emission feature with structure not observed before in other comets or in interstellar silicates. The presence of a strong 11.3 micron peak reported by Bregman and coworkers is confirmed, and evidence is found for additional structure in the band. By comparison with spectra of interplanetary dust particles and laboratory silicates, it is concluded that small crystalline olivine particles are a major component of the silicates in this comet; other silicates (e.g., amorphous or hydrated) must also be present. The identification of crystalline olivine in this part of the spectrum is supported by the observation of four peaks in 20-50 micron airborne spectra of this comet which have also been attributed to olivine.

Campins, Humberto↗
NASA NTRS1994

The 8-13 micron spectra of comets and the composition of silicate grains

We have analyzed the existing spectra of seven comets which show an emission feature at 7.8-13 micrometers. Most have been converted to a common calibration, taking into account the SiO feature in late-type standard stars. The spectra are compared with spectra of the Trapezium, interplanetary dust particles (IDPs), laboratory mineral samples, and small particle emission models. The emission spectra show a variety of shapes; there is no unique 'cometary silicate'. A peak at 11.20-11.25 micrometers, indicative of small crystalline olivine particles, is seen in only three comets of this sample, P/Halley, Bradfield 1987 XXIX, and Levy 1990 XX. The widths of the emission features range from 2.6 to 4.1 micrometers (FWHM). To explain the differing widths and the broad 9.8 micrometers maximum, glassy silicate particles, including both pyroxene and olivine compositions, are the most plausible candidates. Calculations of emission models confirm that small grains of glassy silicate well mixed with carbonaceous material are plausible cometary constituents. No single class of chondritic aggregate IDPs exhibits spectra closely matching the comet spectra. A mixture of IDP spectra, particularly the glass-rich aggregates, approximately matches the spectra of comets P/Halley, Levy, and Bradfield 1987 XXIX. Yet, if comets are simply a mix of IDP types, it is puzzling that the classes of IDPs are so distinct. None of the comet spectra match the spectrum of the Trapezium. Thus, the mineralogy of the cometary silicates is not the same as that of the interstellar medium. The presence of a component of crystalline silicates in comets may be evidence of mixing between high- and low-temperature regions in the solar nebula.

Hanner, Martha S.↗
NASA NTRS2002

Disappearance of 19P/Borrelly's Silicate Feature in 2001 Apparition Is Attributed to Increase in Grain Size

We report on observations and analysis of HIFOGS 10 microns spectrophotometry of short period comet 19P/Borrelly on 2003 October 13, 15 UT at the NASA IRTF. 19P/Borrelly is one of two short period comets, comet 4PIFaye being the other, to have a silicate feature detected. During Borrelly s perihelion passage in 1994 December, a silicate feature was present with a flux-to-continuum ratio of 0.25. Two apparitions later in 2003 October, the silicate feature is absent. Thermal emission modeling using amorphous olivine and amorphous carbon shows that a slight increase in grain size accounts for the disappearance of the silicate feature. Analysis of 19P/Borrelly suggests grain size, and not the absence of olivine minerals, may be responsible for the absence of silicate features in most short period comets. 19P/Borrelly is one of the more active short period comets. However, short period comets as a family are less active than long period comets. Short period comets probably originated in the Kuiper Belt and suffered collisions while in residence in the outer solar system. Upon evolution into orbits that take them through the inner solar system, the surfaces of short period comets are exposed to sunlight through their many perihelion passages. This is in contrast to long period comets which probably originated near Jupiter and were expelled to the Oort cloud where they have existed and been exposed to cosmic ray processing. By studying the grain properties in short period comets and comparing to long period comets, we compare the effects on the grain populations of different parent body evolution histories. Upcoming opportunities to study short and long period comets will be advertised.

Wooden, D. H.↗
NASA NTRS2004

Organic Modification of a Layered Silicate by Co-Ion Exchange of an Alkyl Ammonium and a Mono-Protonated Diamine

Co-Ion exchange of the interlayer cations of a layered silicate with a mono-protonated aromatic diamine and an alkyl ammonium ion into the silicate galleries. The presence of the alkyl ammonium ion provides low oligomer melt viscosity during processing. The presence of the diamine allows chemical reaction between the silicate surface modification and the monomers. This reaction strengthens the polymer silicate interface, and ensures irreversible separation of the individual silicate layers. Improved polymer thermal oxidative stability and mechanical properties are obtained.

Sandi G Campbell↗
NASA NTRS2005

Silicate Inclusions in the Kodaikanal IIE Iron Meteorite

Silicate inclusions in iron meteorites display an astonishing chemical and mineralogical variety, ranging from chondritic to highly fractionated, silica- and alkali-rich assemblages. In spite of this, their origin is commonly considered to be a simple one: mixing of silicates, fractionated or unfractionated, with metal. The latter had to be liquid in order to accommodate the former in a pore-free way which all models accomplish by assuming shock melting. II-E iron meteorites are particularly interesting because they contain an exotic zoo of silicate inclusions, including some chemically strongly fractionated ones. They also pose a formidable conundrum: young silicates are enclosed by very old metal. This and many other incompatibilities between models and reality forced the formulation of an alternative genetic model for irons. Here we present preliminary findings in our study of Kodaikanal silicate inclusions.

Kurat, G.↗
NASA NTRS2006

Grain Growth and Silicates in Dense Clouds

Interstellar silicates are likely to be a part of all grains responsible for visual extinction (Av) in the diffuse interstellar medium (ISM) and dense clouds. A correlation between Av and the depth of the 9.7 micron silicate feature (measured as optical depth, tau(9.7)) is expected if the dust species are well 'mixed. In the di&se ISM, such a correlation is observed for lines of sight in the solar neighborhood. A previous study of the silicate absorption feature in the Taurus dark cloud showed a tendency for the correlation to break down at high Av (Whittet et al. 1988, MNRAS, 233,321), but the scatter was large. We have acquired Spitzer Infrared Spectrograph data of several lines of sight in the IC 5 146, Barnard 68, Chameleon I and Serpens dense clouds. Our data set spans an Av range between 2 and 35 magnitudes. All lines of sight show the 9.7 micron silicate feature. The Serpens data appear to follow the diffuse ISM correlation line whereas the data for the other clouds show a non-linear correlation between the depth of the silicate feature relative to Av, much like the trend observed in the Taurus data. In fact, it appears that for visual extinctions greater than about 10 mag, tau(9.7) begins to level off. This decrease in the growth of the depth of the 9.7 micron feature with increasing Av could indicate the effects of grain growth in dense clouds. In this poster, we explore the possibility that grain growth causes an increase in opacity (Av) without causing a corresponding increase in tau(9.7).

Pendeleton, Yvonne J.↗
NASA NTRS2008

Optical Properties of Astronomical Silicates in the Far-infrared

Correct interpretation of a vast array of astronomical data relies heavily on understanding the properties of silicate dust as a function of wavelength, temperature, and crystallinity. We introduce the QPASI-T (Optical Properties of Astronomical Silicates with Infrared Techniques) project to address the need for high fidelity optical characterization data on the various forms of astronomical dust. We use two spectrometers to provide extinction data for silicate samples across a wide wavelength range (from the near infrared to the millimeter). New experiments are in development that will provide complementary information on the emissivity of our samples, allowing us to complete the optical characterization of these dust materials. In this paper, we present initial results from several materials including amorphous iron silicate, magnesium silicate and silica smokes, over a wide range of temperatures, and discuss the design and operation of our new experiments.

Rinehart, Stephen A,↗
NASA NTRS2009

Identification of an Extremely 180-Rich Presolar Silicate Grain in Acfer 094

Presolar silicate grains have been abundantly identified since their first discovery less than a decade ago [1,2,3]. The O isotopic compositions of both silicate and oxide stardust indicate the vast majority (>90%) condensed around Orich asymptotic giant branch (AGB) stars. Though both presolar phases have average sizes of ~300 nm, grains larger than 1 m are extremely uncommon for presolar silicates. Thus, while numerous isotopic systems have been measured in presolar oxide grains [4], very few isotopic analyses for presolar silicates exist outside of O and Si [2,5]. And still, these measurements suffer from isotopic dilution with surrounding matrix material [6]. We conduct a search for presolar silicates in the primitive carbonaceous chondrite Acfer 094 and in some cases obtain high spatial resolution, high precision isotopic ratios.

Nguyen, A. N.↗
NASA NTRS2009

Amorphous Silicates in Primitive Meteoritic Materials: Acfer 094 and IDPs

The abundance of presolar grains is one measure of the primitive nature of meteoritic materials. Presolar silicates are abundant in meteorites whose matrices are dominated by amorphous silicates such as the unique carbonaceous chondrite Acfer 094. Presolar silicates are even more abundant in chondritic-porous interplanetary dust particles (CP-IDPs). Amorphous silicates in the form of GEMS (glass with embedded metal and sulfides) grains are a major component of CP IDPs. We are studying amorphous silicates in Acfer 094 matrix in order to determine whether they are related to the GEMS grains in CPIDPs

Keller, L. P.↗
NASA NTRS2009

Calculation of Oxygen Fugacity in High Pressure Metal-Silicate Experiments and Comparison to Standard Approaches

Calculation of oxygen fugacity in high pressure and temperature experiments in metal-silicate systems is usually approximated by the ratio of Fe in the metal and FeO in the silicate melt: (Delta)IW=2*log(X(sub Fe)/X(sub FeO)), where IW is the iron-wustite reference oxygen buffer. Although this is a quick and easy calculation to make, it has been applied to a huge variety of metallic (Fe- Ni-S-C-O-Si systems) and silicate liquids (SiO2, Al2O3, TiO2, FeO, MgO, CaO, Na2O, K2O systems). This approach has surely led to values that have little meaning, yet are applied with great confidence, for example, to a terrestrial mantle at "IW-2". Although fO2 can be circumvented in some cases by consideration of Fe-M distribution coefficient, these do not eliminate the effects of alloy or silicate liquid compositional variation, or the specific chemical effects of S in the silicate liquid, for example. In order to address the issue of what the actual value of fO2 is in any given experiment, we have calculated fO2 from the equilibria 2Fe (metal) + SiO2 (liq) + O2 = Fe2SiO4 (liq).

Righter, K.↗
NASA NTRS2010

High Pressure/Temperature Metal Silicate Partitioning of Tungsten

The behavior of chemical elements during metal/silicate segregation and their resulting distribution in Earth's mantle and core provide insight into core formation processes. Experimental determination of partition coefficients allows calculations of element distributions that can be compared to accepted values of element abundances in the silicate (mantle) and metallic (core) portions of the Earth. Tungsten (W) is a moderately siderophile element and thus preferentially partitions into metal versus silicate under many planetary conditions. The partitioning behavior has been shown to vary with temperature, silicate composition, oxygen fugacity, and pressure. Most of the previous work on W partitioning has been conducted at 1-bar conditions or at relatively low pressures, i.e. <10 GPa, and in two cases at or near 20 GPa. According to those data, the stronger influences on the distribution coefficient of W are temperature, composition, and oxygen fugacity with a relatively slight influence in pressure. Predictions based on extrapolation of existing data and parameterizations suggest an increased pressured dependence on metal/ silicate partitioning of W at higher pressures 5. However, the dependence on pressure is not as well constrained as T, fO2, and silicate composition. This poses a problem because proposed equilibration pressures for core formation range from 27 to 50 GPa, falling well outside the experimental range, therefore requiring exptrapolation of a parametereized model. Higher pressure data are needed to improve our understanding of W partitioning at these more extreme conditions.

Shofner, G. A.↗
NASA NTRS2012

Search for Large Presolar Silicate Grains in the QUE 99177 CR Chondrite

Silicates are among the most abundant pre-solar grain type, and their diverse chemical and isotopic compos-tions preserve detailed constraints on their stellar origins, condensation conditions, and nucleosynthetic and interstellar processes. Yet, owing to their small sizes, relatively few grains have been measured for isotopic compositions besides O and Si, and their mineralogy is poorly characterized. The average grain size (approx 270 nm) limits the number of analyses that can be conducted on a given grain, and their identification among solar system silicates introduces contaminating signal. These difficulties can be overcome by identifying large presolar silicate grains. However, such grains are very rare and only two approx 1 micron grains have been discovered. We are conducting a dedicated search for large presolar silicates in size-separated QUE 99177 matrix material. This primitive meteorite has among the highest abundance of presolar silicates

Nguyen, A. N.↗
NASA NTRS2013

The W-W02 Oxygen Fugacity Buffer at High Pressures and Temperatures: Implications for f02 Buffering and Metal-silicate Partitioning

Oxygen fugacity (fO2) controls multivalent phase equilibria and partitioning of redox-sensitive elements, and it is important to understand this thermodynamic parameter in experimental and natural systems. The coexistence of a metal and its oxide at equilibrium constitutes an oxygen buffer which can be used to control or calculate fO2 in high pressure experiments. Application of 1-bar buffers to high pressure conditions can lead to inaccuracies in fO2 calculations because of unconstrained pressure dependencies. Extending fO2 buffers to pressures and temperatures corresponding to the Earth's deep interior requires precise determinations of the difference in volume (Delta) V) between the buffer phases. Synchrotron x-ray diffraction data were obtained using diamond anvil cells (DAC) and a multi anvil press (MAP) to measure unit cell volumes of W and WO2 at pressures and temperatures up to 70 GPa and 2300 K. These data were fitted to Birch-Murnaghan 3rd-order thermal equations of state using a thermal pressure approach; parameters for W are KT = 306 GPa, KT' = 4.06, and αKT = 0.00417 GPa K-1. Two structural phase transitions were observed for WO2 at 4 and 32 GPa with structures in P21/c, Pnma and C2/c space groups. Equations of state were fitted for these phases over their respective pressure ranges yielding the parameters KT = 190, 213, 300 GPa, KT' = 4.24, 5.17, 4 (fixed), and αKT = 0.00506, 0.00419, 0.00467 GPa K-1 for the P21/c, Pnma and C2/c phases, respectively. The W-WO2 buffer (WWO) was extended to high pressure by inverting the W and WO2 equations of state to obtain phase volumes at discrete pressures (1-bar to 100 GPa, 1 GPa increments) along isotherms (300 to 3000K, 100 K increments). The slope of the absolute fO2 of the WWO buffer is positive with increasing temperature up to approximately 70 GPa and is negative above this pressure. The slope is positive along isotherms from 1000 to 3000K with increasing pressure up to at least 100 GPa. The WWO buffer is at a higher fO2 than the IW buffer at pressures lower than 40 GPa, and the magnitude of this difference decreases at higher pressures. This qualitatively indicates an increasingly lithophile character for W at higher pressures. The WWO buffer was quantitatively applied to W metal-silicate partitioning by using the WWO-IW buffer difference in combination with literature data on W metal-silicate partitioning to model the exchange coefficient (KD) for the Fe-W exchange reaction. This approach captures the pressure dependence of W metal-silicate partitioning using the WWO-IW buffer difference and models the activities of the components in the silicate and metallic phases using an expression of the Gibbs excess energy of mixing. Calculation of KD along a peridotite liquidus predicts a decrease in W siderophility at higher pressures that supports the qualitative behavior predicted by the WWO-IW buffer difference, and agrees with findings of others. Comparing the competing effects of temperature and pressure on W metal-silicate partitioning, our results indicate that pressure exerts a greater effect.

Shofner, G. A.↗
NASA NTRS2016

Laboratory Analysis of Silicate Stardust Grains of Diverse Stellar Origins

Silicate dust is ubiquitous in a multitude of environments across the cosmos, including evolved oxygen-rich stars, interstellar space, protoplanetary disks, comets, and asteroids. The identification of bona fide silicate stardust grains in meteorites, interplanetary dust particles, micrometeorites, and dust returned from comet Wild 2 by the Stardust spacecraft has revolutionized the study of stars, interstellar space, and the history of dust in the Galaxy. These stardust grains have exotic isotopic compositions that are records of nucleosynthetic processes that occurred in the depths of their now extinct parent stars. Moreover, the chemical compositions and mineralogies of silicate stardust are consequences of the physical and chemical nature of the stellar condensation environment, as well as secondary alteration processes that can occur in interstellar space, the solar nebula, and on the asteroid or comet parent body in which they were incorporated. In this talk I will discuss our use of advanced nano-scale instrumentation in the laboratory to conduct coordinated isotopic, chemical, and mineralogical analyses of silicate stardust grains from AGB stars, supernovae, and novae. By analyzing the isotopic compositions of multiple elements in individual grains, we have been able to constrain their stellar sources, explore stellar nucleosynthetic and mixing processes, and Galactic chemical evolution. Through our mineralogical studies, we have found these presolar silicate grains to have wide-ranging chemical and mineral characteristics. This diversity is the result of primary condensation characteristics and in some cases secondary features imparted by alteration in space and in our Solar System. The laboratory analysis of actual samples of stars directly complements astronomical observations and astrophysical models and offers an unprecedented level of detail into the lifecycles of dust in the Galaxy.

Nguyen, Ann N.↗
NASA NTRS2020

Calorimetric Measurements of the Thermodynamic Properties of RE-Silicate Coating Materials

Thermodynamic quantities of coatings materials and siliceous debris-induced corrosion products are crucial to understand in order to develop mitigation strategies necessary to improve the durability of gas-turbine engines. Siliceous induced corrosion can occur when debris consisting mainly of CaO-MgO-Al2O3-SiO2 (CMAS) is ingested by aircraft engines during and after take-off, which sticks to hot surfaces and forms calcium rare-earth silicate oxyapatites. In this work, high-temperature oxide melt drop solution calorimetry (HT drop solution calorimetry) was used to obtain the enthalpies of formation for RE silicate (RE2Si2O7, RE2SiO5 where RE = Yb, Er, Y, Dy, Nd, Lu and Gd) environmental barrier coatings (EBCs) and the calcium RE silicate oxyapatite Ca2RE8(SiO4)6O2 (RE = Yb, Er, Y, Dy, Nd, Gd and Sm) corrosion products. Trends in the enthalpy of formation as a function of the ionic potential of the rare-earth cations in their related crystallographic sites are discussed.

Costa, Gustavo↗
NASA NTRS2020

Coordinated NanoSIMS and TEM Analysis of a Large 26Mg-Rich AGB Silicate from the Meteorite Hills 00426 CR2 Chondrite

Silicates are one of the most abundant presolar phases around evolved stars, in the inter-stellar medium (ISM), and in our Solar System. These grains afford the opportunity for O, Si, Mg, Fe, and Ca isotopic analyses to constrain stellar nucleosynthetic and mixing processes, and Galactic chemical evolution (GCE). While Mg and Fe isotopic studies have been successfully conducted on presolar silicates, isotopic analyses beyond O and Si are often hampered by the small grain sizes (average ~250 nm). This also makes coordinated mineral and chemical characterization challenging. These studies provide insight into the dust condensation conditions as well as subsequent alteration in the ISM and/or the Solar System. TEM studies of presolar silicates have shown that they are much more mineralogically and chemically diverse than other presolar phases [1 and references therein]. Large (>500nm) presolar silicate grains are rare, but they allow for detailed isotopic, mineral, and chemical characterization. We identified a large presolar silicate grain in the MET 00426 CR2 chondrite and report the O, Si, Mg, and Fe isotopic compositions and TEM study of this grain.

Nguyen, A. N.↗