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1.
We report the development of a new analytical system allowing the fully automated measurement of isotopic ratios in micrometer-sized particles by secondary ion mass spectrometry (SIMS) in a Cameca ims-6f ion microprobe. Scanning ion images and image processing algorithms are used to locate individual particles dispersed on sample substrates. The primary ion beam is electrostatically deflected to and focused onto each particle in turn, followed by a peak-jumping isotopic measurement. Automatic measurements of terrestrial standards indicate similar analytical uncertainties to traditional manual particle analyses (e.g., ∼3‰/amu for Si isotopic ratios). We also present an initial application of the measurement system to obtain Si and C isotopic ratios for ∼3300 presolar SiC grains from the Murchison CM2 carbonaceous chondrite. Three rare presolar Si3N4 grains were also identified and analyzed. Most of the analyzed grains were extracted from the host meteorite using a new chemical dissolution procedure. The isotopic data are broadly consistent with previous observations of presolar SiC in the same size range (∼0.5-4 μm). Members of the previously identified SiC AB, X, Y, and Z subgroups were identified, as was a highly unusual grain with an extreme 30Si enrichment, a modest 29Si enrichment, and isotopically light C. The stellar source responsible for this grain is likely to have been a supernova. Minor differences in isotopic distributions between the present work and prior data can be partially explained by terrestrial contamination and grain aggregation on sample mounts, though some of the differences are probably intrinsic to the samples. We use the large new SiC database to explore the relationships between three previously identified isotopic subgroups—mainstream, Y, and Z grains—all believed to originate in asymptotic giant branch stars. The isotopic data for Z grains suggest that their parent stars experienced strong CNO-cycle nucleosynthesis during the early asymptotic giant branch phase, consistent with either cool bottom processing in low-mass (M < 2.3M⊙) parent stars or hot-bottom burning in intermediate-mass stars (M > 4M⊙). The data provide evidence for a sharp threshold in metallicity, above which SiC grains form with much higher 12C/13C ratios than below. Above this threshold, the fraction of grains with relatively high 12C/13C decreases exponentially with increasing 29Si/28Si ratio. This result indicates a sharp increase in the maximum mass of SiC parent stars with decreasing metallicity, in contrast to expectations from Galactic chemical evolution theory.  相似文献   

2.
We report isotopic ratio measurements of small SiC and Si3N4 grains, with special emphasis on presolar SiC grains of type Z, and new nucleosynthesis models for 26Al/27Al and the Ti isotopic ratios in asymptotic giant branch (AGB) stars. With the NanoSIMS we analyzed 310 SiC grains from Murchison (carbonaceous CM2 chondrite) separate KJB (diameters 0.25-0.45 μm) and 153 SiC grains from KJG (diameters 1.8-3.7 μm), 154 SiC and 23 Si3N4 grains from Indarch (enstatite EH4 chondrite) separate IH6 (diameters 0.25-0.65 μm) for their C and N isotopic compositions, 549 SiC and 142 Si3N4 grains from IH6 for their C and Si isotopic compositions, 13 SiC grains from Murchison and 66 from Indarch for their Al-Mg compositions, and eight SiC grains from Murchison and 10 from Indarch for their Ti isotopic compositions. One of the original objectives of this effort was to compare isotopic analyses with the NanoSIMS with analyses previously obtained with the Cameca IMS 3f ion microprobe. Many of the Si3N4 grains from Indarch have isotopic anomalies but most of these apparently originate from adjacent SiC grains. Only one Si3N4 grain, with 13C and 14N excesses, has a likely AGB origin. The C, N, and Si isotopic data show that the percentage of SiC grains of type Y and Z increase with decreasing grain size (from ∼1% for grains >2 μm to ∼5-7% for grains of 0.5 μm), providing an opportunity for isotopic analyses in these rare grains. Our measurements expand the number of Al-Mg analyses on SiC Z grains from 4 to 23 and the number of Ti analyses on Z grains from 2 to 11. Inferred26Al/27Al ratios of Z grains are in the range found in mainstream and Y grains and do not exceed those predicted by models of AGB nucleosynthesis. Cool bottom processing (CBP) has been invoked to explain the low 12C/13C ratios of Z grains, but this process apparently does not lead to increased 26Al production in the parent stars of these grains. This finding is in contrast to presolar oxide grains where CBP is needed to explain their high 26Al/27Al ratios. The low 46,47,49Ti/48Ti ratios found in Z grains and their correlation with low 29Si/28Si ratios extend the trend seen in mainstream grains and confirm an origin in low-metallicity AGB stars. The relatively large excesses in 30Si and 50Ti in Z grains are predicted by our models to be the result of increased production of these isotopes by neutron-capture nucleosynthesis in low-metallicity AGB stars. However, the predicted excesses in 50Ti (and 49Ti) are much larger than those found. Even lowering the strength of the 13C pocket cannot solve this discrepancy in a consistent way.  相似文献   

3.
Silicon carbide (SiC) is a particularly interesting species of presolar grain because it is known to form on the order of a hundred different polytypes in the laboratory, and the formation of a particular polytype is sensitive to growth conditions. Astronomical evidence for the formation of SiC in expanding circumstellar atmospheres of asymptotic giant branch (AGB) carbon stars is provided by infrared (IR) studies. However, identification of the crystallographic structure of SiC from IR spectra is controversial. Since >95% of the presolar SiC isolated from meteorites formed around carbon stars, a determination of the structure of presolar SiC is, to first order, a direct determination of the structure of circumstellar SiC. We therefore determined the polytype distribution of presolar SiC from the Murchison CM2 carbonaceous meteorite using analytical and high-resolution transmission electron microscopy (TEM). High-resolution lattice images and electron diffraction of 508 individual SiC grains demonstrate that only two polytypes are present, the cubic 3C (β-SiC) polytype (79.4% of population by number) and the hexagonal 2H (α-SiC) polytype (2.7%). Intergrowths of these two polytypes are relatively abundant (17.1%). No other polytypes were found. A small population of one-dimensionally disordered SiC grains (0.9%), whose high density of stacking faults precluded classification as any polytype, was also observed. The presolar origin of 2H α-SiC is unambiguously established by tens-of-nanometers-resolution secondary ion mass spectroscopy (NanoSIMS). Isotopic maps of a TEM-characterized 2H α-SiC grain exhibit non-solar isotopic compositions of 12C/13C = 64 ± 4 and 14N/15N = 575 ± 24. These measurements are consistent with mainstream presolar SiC thought to originate in the expanding atmospheres of AGB carbon stars. Equilibrium condensation calculations together with inferred mineral condensation sequences predict relatively low SiC condensation temperatures in carbon stars. The laboratory observed condensation temperatures of 2H and 3C SiC are generally the lowest of all SiC polytypes and fall within the predictions of the equilibrium calculations. These points account for the occurrence of only 2H and 3C polytypes of SiC in circumstellar outflows. The 2H and 3C SiC polytypes presumably condense at different radii (i.e., temperatures) in the expanding stellar atmospheres of AGB carbon stars.  相似文献   

4.
With a new type of ion microprobe, the NanoSIMS, we determined the oxygen isotopic compositions of small (<1μm) oxide grains in chemical separates from two CM2 carbonaceous meteorites, Murray and Murchison. Among 628 grains from Murray separate CF (mean diameter 0.15 μm) we discovered 15 presolar spinel and 3 presolar corundum grains, among 753 grains from Murray separate CG (mean diameter 0.45 μm) 9 presolar spinel grains, and among 473 grains from Murchison separate KIE (mean diameter 0.5 μm) 2 presolar spinel and 4 presolar corundum grains. The abundance of presolar spinel is highest (2.4%) in the smallest size fraction. The total abundance in the whole meteorite is at least 1 ppm, which makes spinel the third-most abundant presolar grain species after nanodiamonds (if indeed a significant fraction of them are presolar) and silicon carbide. The O-isotopic distribution of the spinel grains is very similar to that of presolar corundum, the only statistically significant difference being that there is a larger fraction of corundum grains with large 17O excesses (17O/16O > 1.5 × 10−3), which indicates parent stars with masses between 1.8 and 4.5 M⊙.  相似文献   

5.
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6.
We report the results of a study of 81 micrometer-sized presolar SiC grains in the size range 0.5-2.6 μm from the Murchison (CM2) carbonaceous chondrite. We describe a simple, nondestructive physical disaggregation technique used to isolate the grains while preserving them in their pristine state, as well as the scanning electron microscopy energy-dispersive X-ray mapping procedure used to locate them.Nine-tenths of the pristine SiCs are bounded by one or more planar surfaces consistent with cubic (3C polytype) crystal faces based on manifest symmetry elements. In addition, multiple polygonal depressions (generally <100 nm deep) are observed in more than half of these crystal faces, and these possess symmetries consistent with the structure of the 3C polytype of SiC. By comparison of these features with the surface features present on heavily etched presolar SiC grains from Murchison separate KJG, we show that the polygonal depressions on pristine grains are likely primary growth features. The etched SiCs have high densities of surface pits, in addition to polygonal depressions. If these pits are etched linear defects in the SiC, then defect densities are quite high (as much as 108 -109/cm2), about 103-104 times higher than in typical synthetic SiCs. The polygonal depressions on crystal faces of pristine grains, as well as the high defect densities, indicate rapid formation of presolar SiC.No other primary minerals are observed to be intergrown with or overgrown on the pristine SiCs, so the presence of overgrowths of other minerals cannot be invoked to account for the survival of presolar SiC in the solar nebula. We take the absence of other primary condensates to indicate that further growth or back-reaction with the gas became kinetically inhibited as the gas-phase densities in the expanding asymptotic giant branch (AGB) stellar atmospheres (in which most of the grains condensed) became too low. However, we did observe an oxygen peak in the X-ray spectra of most pristine grains, implying silica coatings of as much as several tens of nm thickness, perhaps due to oxidation of the SiC in the solar nebula.We see little or no evidence on the pristine grains of the surface sputtering or cratering that are predicted theoretically to occur in the interstellar medium (ISM) due to supernova shocks. A possible implication is that the grains may have been protected during their residence in the ISM by surface coatings, including simple ices. Residues of such coatings may indeed be present on some pristine SiCs, because many (60%) are coated with an apparently amorphous, possibly organic phase. However, at present we do not have sufficient data on the coatings to draw secure inferences as to their nature or origin.A few irregular pristine SiCs, either fragments produced by regolith gardening on the Murchison parent body or by grain-grain collisions in the ISM, were also observed.  相似文献   

7.
A new microscale oxybarometer for solar system basaltic glasses, based on vanadium K-edge X-ray absorption near edge structure (XANES) spectroscopy, is described. Vanadium is unique among abundant elements in siliceous materials in that it can potentially occur in nature in four valence states: V2+, V3+, V4+ and V5+. Consequently, the vanadium redox system is a robust oxybarometer covering at least six orders of magnitude in buffer-relative oxygen fugacity. The method was calibrated using synthetic glass standards produced under known fO2 and temperature conditions. Correction for temperature differences among standards and unknowns was quantified using microXANES data for isobaric synthetic glass couples. Application of the method to lunar, martian, and terrestrial glasses yielded fO2 estimates from 1.6 log units more reduced than the iron-wüstite (IW) buffer (IW-1.6) for lunar glasses, to IW + 4.0 for terrestrial glass inclusions. The martian and terrestrial results are in good agreement with previous estimates by other methods. The inferred fO2 values for lunar pyroclastic glasses are ∼0.5 log unit more reduced than previous estimates, but the differences are comparable to analytical uncertainties. Micro-extended X-ray absorption fine structure spectra were consistent with the valence states determined by microXANES and provided additional constraints on vanadium site geometry. These results demonstrate the value of this new oxybarometer, which can be applied nondestructively to individual grains in conventional thin sections with ∼ micrometer resolution and ∼100 ppm elemental sensitivity.  相似文献   

8.
High pressure experiments have been performed in the systems Mg2SiO4-C-O-H and Mg2SiO4-K2CO3-C at 6.3 GPa and 1200 to 1600 °C using a split-sphere multi-anvil apparatus. In the Mg2SiO4-C-O-H system the composition of fluid was modeled by adding different amounts of water and stearic acid. The fO2 was controlled by the Mo-MoO2 or Fe-FeO oxygen buffers. Several experiments in the Mg2SiO4-C-O-H system and all experiments in the Mg2SiO4-K2CO3-C system have been conducted without buffering the fO2. Forsterite in the system Mg2SiO4-K2CO3-C does not reveal OH absorption bands in the IR spectra, while forsterite coexisting with carbon-bearing fluid and silicate melt at logfO2 from FMQ-2 to FMQ-5 (from 2 to 5 log units below fayalite-magnetite-quartz oxygen buffer) contains 800-1850 wt. ppm H2O. The maximum concentrations were detected at 1400 °C and FMQ-3.5. We observed an increase in the solidus temperature in the system Mg2SiO4-C-O-H from 1200 to above 1600 °C with log fO2 decreasing from FMQ-2 to FMQ-5. The increase of the solidus temperature and the broadening of the stability field of the H2O-H2-CH4 subsolidus fluid phase at 1400-1600 °C explain the high H2O storage capacity of forsterite relative to that crystallized from carbon-free, oxidized, hydrous, silicic melt. At temperatures above 1400 °C liquidus forsterite precipitated along with diamond from oxidized (FMQ-1) carbonate-silicate melt and from silicate melt dissolving the moderately reduced C-O-H fluid (from FMQ-2 to FMQ-3.5). Formation of diamond was not detected under ultra-reduced conditions (FMQ-5) at 1200-1600 °C. Olivine co-precipitating with diamond from dry carbonate-silicate or hydrous-silicic fluid/melt can provide information on the H2O contents and speciation of the diamond-forming media in the mantle. The conditions for minimum post-crystallization alteration of olivine and its hydrogen content are discussed.  相似文献   

9.
A calcite-marble containing gem-quality ruby is exposed in the Hunza Valley, northwestern part of the Karakoram mountains, Pakistan zone of Kashmir. The marble forms concordant intercalations within sillimanite- and garnet-bearing biotite-plagioclase gneisses and mica schists. The metamorphic sequence is cut by discordant aplite and pegmatite dikes. The following mineral assemblages are recognized in the marble:1) Calcite+corundum+phlogopite±margarite±sheridanite±Al-rich pargasite±anorthite (An 96.7),2) calcite+spinel±corundum+phlogopite+sheridanite.Microprobe analyses are given for the essential minerals including corundum (ruby) and three different colour varieties of spinel. On the basis of recent experimental data, especially in the system CaO - Al2O3 - SiO2 - H2O -CO2 (and related subsystems), we assume that, during the regional metamorphism, temperatures of about 600 – 620°C and a water vapour pressure of about 6 kb were realized in part of the Hunza area. The gas phase must have contained roughly 20 mole-% of CO2. Thus the total fluid pressure may have reached about 7 kb. Presumably, temperatures increased in northwest direction, perhaps up to about 700°C. The estimated P-T conditions are consistent with a geothermal gradient of about 25°C/km.  相似文献   

10.
We report the results of coordinated ion microprobe and transmission electron microscope (TEM) studies of presolar graphites from the KE3 separate (1.65-1.72 g/cm3) of the Murchison CM2 meteorite. Isotopic analysis of individual graphites (1-12 μm) with the ion microprobe shows many to have large 18O excesses combined with large silicon isotopic anomalies, indicative of a supernova (SN) origin. Transmission electron microscopy (TEM) of ultramicrotome slices of these SN graphites revealed a high abundance (25-2400 ppm) of internal titanium carbides (TiCs), with a single graphite in some cases containing hundreds of TiCs. Isotopic compositions of individual TiCs by nanoscale resolution secondary ion mass spectrometry (NanoSIMS) confirmed their presolar origin. In addition to TiCs, composite TiC/Fe grains (TiCs with attached iron-nickel subgrains) and solitary kamacite internal grains were found. In the composite grains, the attached iron phase (kamacite [0-24 at. % Ni] or taenite [up to 60 at. % Ni]) was epitaxially grown onto one or more TiC faces. In contrast to the denser Murchison KFC1 graphites, no Zr-Ti-Mo carbides were observed. The average TiC diameters were quite variable among the SN graphites, from 30 to 232 nm, and were generally independent of the host graphite size. TiC grain morphologies ranged from euhedral to anhedral, with the grain surfaces exhibiting variable degrees of corrosion, and sometimes partially amorphous rims (3 to 15 nm thick). Partially amorphous rims of similar thickness were also observed on some solitary kamacite grains. We speculate that the rims on the internal grains are most plausibly the result of atom bombardment caused by drift of grains with respect to the ambient gas, requiring relative outflow speeds ∼100 km/s (i.e., a few percent of the SN mass outflow speed).Energy dispersive X-ray spectrometry (EDXS) of TiCs revealed significant V in solid solution, with an average V/Ti ratio over all TiCs of ∼83% of the solar value of 0.122. Significant variations about the mean V/Ti ratio were also seen among TiCs in the same graphite, likely indicating chemical equilibration with the surrounding gas over a range of temperatures. In general, the diversity in internal TiC properties suggests that TiCs formed first and had substantially diverse histories before incorporation into the graphite, implying some degree of turbulent mixing in the SN outflows.In most graphites, there is a decrease in the number density of TiCs as a function of increasing radial dis- tance, caused by either preferential depletion of TiCs from the gas or an acceleration of graphite growth with decreasing ambient temperature. In several graphites, TiCs showed a trend of larger V/Ti ratios with increasing distance from the graphite center, an indication of progressive equilibration with the surrounding gas before they were sequestered in the graphites. In all but one graphite, no trend was seen in the TiC size vs. distance from the graphite center, implying that appreciable TiC growth had effectively stopped before the graphites formed, or else that graphite growth was rapid compared to TiC growth. Taken together, the chemical variations among internal grains as well as the presence of partially amorphous rims and epitaxial Fe phases on some TiCs clearly indicate that the phase condensation sequence was TiC, followed by the iron phases (only found in some graphites) and finally graphite. Since graphite typically condenses at a higher temperature than iron at low pressures (<10−3 bars) in a gas with C > O and otherwise solar composition, the observed condensation sequence implies a relative iron enrichment in the gas or greater supersaturation of graphite relative to iron.The TEM observations allow inferences to be made about the physical conditions in the gas from which the grains condensed. Given the TiC sizes and abundances, the gas was evidently quite dusty. From the observed TiC size range of ∼20 nm to ∼500 nm (assuming ∼1 yr growth time and T ∼ 1800°K), we infer minimum Ti number densities in the gas to be ∼7 × 104 to ∼2 × 106 atoms/cc, respectively. Although the gas composition is clearly not solar, for scale, these number densities would correspond to a pressure range of ∼0.2 μbar to ∼5.0 μbar in a gas of solar composition. They also correspond to minimum TiC grain number densities of ∼3 × 10−4 to ∼0.2 grains/cc, assuming complete condensation of Ti in TiC. We estimate the maximum ratio of mean TiC grain separation distance in the gas to grain diameter from the Ti number densities as ∼3 × 105 to ∼1 × 106.  相似文献   

11.
Study on presolar grains including diamond,silicon carbide,graphite,silicon nitrite(Si3N4),coundum and spinel isolated from meteorites is summarized in this paper.Except for nanometer-sized diamond,the other grains are micrometers to submicrometers in size.The presolar grains survived mainly in the fine-grained matrix of primitive chondrites and were isolated by chemical treatments.Diamond contains Xe isotopes(Xe-HL),typically produced in p-and r-processes,probably formed in supernovae.Mainstream silicon carbides are enriched in ^29,30Si and ^13C,but depleted in ^15N.They also contain various s-process products,consistent with calculations of AGB stars.Other silicon carbides exhibit much larger isotopic anomalies and are classified as groups X,Y,Z and AB.Among them,group X of SiC is characterized by enrichment of ^28Si and daughter isotopes of various short-lived nuclides,suggesting an origin from supernovae.Graphite can be divided into four density fractions with distince isotopic compositions.They may form in AGB stars,novae and supernovae,respctively,Si3N4 is similar to X-SiC in isotopic composition.Corundum is classified as four groups based on theid oxygen isotopic compositions.AGB and red giang stare are possible sources for the oxide.More comprehensive study of presolar grains,especially discovery of the other types of oxides and silicates,isotopic analyses of individual submicrometer-sized grains and distribution of presolar grains among various chemical groups and petropaphic types of chondrites will provide new information on nucleosynthesis,stellar evolution and formation of the solar nebula.  相似文献   

12.
Barium isotopic compositions of single 2.3-5.3 μm presolar SiC grains from the Murchison meteorite were measured by resonant ionization mass spectrometry. Mainstream SiC grains are enriched in s-process barium and show a spread in isotopic composition from solar to dominantly s-process. In the relatively coarse grain size fraction analyzed, there are large grain-to-grain variations of barium isotopic composition. Comparison of single grain data with models of nucleosynthesis in asymptotic giant branch (AGB) stars indicates that the grains most likely come from low mass carbon-rich AGB stars (1.5 to 3 solar masses) of about solar metallicity and with approximately solar initial proportions of r- and s-process isotopes. Measurements of single grains imply a wide variety of neutron-to-seed ratios, in agreement with previous measurements of strontium, zirconium and molybdenum isotopic compositions of single presolar SiC grains.  相似文献   

13.
The dissolution and growth of uranophane [Ca(UO2)2(SiO3OH)2·5H2O] have been examined in Ca- and Si-rich test solutions at low temperatures (20.5 ± 2.0 °C) and near-neutral pH (∼6.0). Uranium-bearing experimental solutions undersaturated and supersaturated with uranophane were prepared in matrices of ∼10−2 M CaCl2 and ∼10−3 M SiO2(aq). The experimental solutions were reacted with synthetic uranophane and analyzed periodically over 10 weeks. Interpretation of the aqueous solution data permitted extraction of a solubility constant for the uranophane dissolution reaction and standard state Gibbs free energy of formation for uranophane ( kJ mol−1).  相似文献   

14.
Solubility experiments for nitrogen and noble gases (Ar and Ne) in silicate melts were conducted using two experimental configurations: one was conducted at 1 atmospheric pressure, T =1300°C and oxygen fugacity (fO2) of IW + 0.9 (i.e., 0.9 log units higher than the iron-wüstite buffer) and the other at high pressures (Ptotal ∼ 2 × 108 Pa), 1500°C and fO2 ∼ IW + 6. For the former experiment, isotopically labeled-nitrogen (15N15N-enriched) was used to distinguish dissolved nitrogen from contaminating atmospheric or organic nitrogen and to examine dissolution mechanisms of nitrogen in silicate melts. The results obtained for the two series of experiments are consistent with each other, suggesting that Henry's law is satisfied for fN2 of up to ∼250 atm (2.5 × 107 Pa). The results are also consistent with our earlier results (Miyazaki et al., 1995) obtained at highly oxidizing conditions (fO2 ∼ IW + 10). All these results support physical dissolution of nitrogen as N2 molecules in silicate melts for fO2 from ∼IW + 10 down to ∼IW. The observed solubility (Henry's constant) of nitrogen (3-5 × 10−9 mol/g/atm) is comparable to that of Ar (2-4 × 10−9 mol/g/atm), and much lower than that of Ne (11-14 × 10−9 mol/g/atm) at 1300°C. A preliminary experiment was also performed for partitioning of nitrogen and noble gases between clinopyroxene (cpx) and basaltic melt using a piston cylinder-type apparatus at 1.5 GPa and at 1270 to 1350°C. The obtained cpx/melt partition coefficient of nitrogen is 0.06, slightly lower than those of noble gases (∼0.1 for Ne to Xe), suggesting that nitrogen is as incompatible as or even slightly more incompatible than noble gases. The present results imply that a large nitrogen/Ar fractionation would not be produced by magmatic processes. Therefore, the two orders of magnitude difference between the N2/36Ar ratios in the Earth's atmosphere (∼104) and that in the mantle (∼106) must be explained by some other processes, such as incomplete segregation of metal blobs into the core and their later oxidation.  相似文献   

15.
Silicate inclusions in IAB irons and related winonaite meteorites have textures, mineralogies and mineral chemistries that indicate a complex formation history of heating, followed by brecciation and metamorphism. Using olivine-orthopyroxene-chromite assemblages in five IAB iron silicate inclusions (Caddo County, Campo del Cielo, Copiapo, Lueders, and Udei Station) and one winonaite (Winona), we calculated closure temperatures and oxygen fugacities for these meteorites. Calculated olivine-chromite Fe-Mg exchange temperatures are compared to two-pyroxene temperatures. Olivine-chromite closure temperatures range from ∼590°C to ∼700°C, while two-pyroxene temperatures range from ∼900°C to ∼1200°C. Oxygen fugacities of these meteorites, determined for the first time in this study, range from 2.3 to 3.2 log units below the Fe-FeO buffer and define a line between the Fe-FeO and Cr-Cr2O3 buffers. Highly variable temperatures were experienced by these rocks on the hand sample, and sometimes even the thin section, scale consistent with the idea that the winonaite-IAB iron parent body experienced collisional fragmentation and reassembly after peak temperatures were reached. Although modest reduction likely occurred during cooling, the oxygen fugacities and mineral compositions recorded at peak metamorphic temperatures suggest that the chondritic precursor for this parent body was initially more reduced than ordinary chondrites.  相似文献   

16.
We have investigated the presolar grain inventories of two CR chondrites, QUE 99177 and MET 00426, which are less altered than most members of this meteorite group. Both meteorites contain high abundances of O-anomalous presolar grains, with concentrations of 220 ± 40 and 160 ± 30 ppm for QUE 99177 and MET 00426, respectively. The presolar grain inventories are dominated by ferromagnesian silicates with group 1 oxygen isotopic compositions, indicative of origins in low mass red giant or asymptotic giant branch stars. Grains with pyroxene-like compositions are somewhat more common than those with olivine-like compositions, but most grains are non-stoichiometric with compositions intermediate between these two phases, consistent with recent work suggesting that amorphous interstellar silicates have stoichiometries between olivine and pyroxene type silicates. Although structural data are not available, one grain contains only Si and O, and has a stoichiometry consistent with SiO2.Our presolar grains are much more Fe-rich than predicted by astronomical observations. Although secondary alteration may play a role in enhancing the Fe contents of presolar grains, it seems unlikely that the large and ubiquitous Fe enrichments observed in the grains from this study can be due only to secondary processing, particularly given the highly primitive nature of these two meteorites. Grain condensation in the stellar outflows where these grains formed likely proceeded under rapidly changing kinetic conditions that may have enhanced the incorporation of Fe into the grains over that expected based on equilibrium condensation theory.Both QUE 99177 and MET 00426 appear to contain unusually low abundances of oxide grains and have higher silicate/oxide ratios than other primitive meteorites analyzed to date. We explore various possibilities for this discrepancy, but note that most scenarios are not likely to result in the preferential destruction of oxides relative to silicates. Thus, the highest silicate/oxide ratios, such as those observed in the CR chondrites, should reflect the true initial proportions of presolar silicate and oxide grains in the parent molecular cloud from which the solar nebula evolved.  相似文献   

17.
Summary Phase fields intersected by three joins in the System CaO-MgO-SiO2-CO2-H2O at 2 kbar were investigated experimentally to determine the melting relationships and the sequences of crystallization of liquids co-precipitating silicate minerals and carbonates. These joins connect SiO2 to three mixtures of CaCO3-MgCO3-Mg(OH)2 with compositions on the primary îield for calcite, between the composition CaCO3 and the low-temperature (650°C eutectic liquid co-precipitating calcite, dolomite and periclase. In the pseudo-quaternary tetrahedron calcite-magnesite-brucite-diopside, two of the significant reactions found are: (1) a eutectic at 650°C, calcite + dolomite + periclase + forsterite + vapor = liquid, and (2) a peritectic at 1038°Cwhich is either calcite + åkermanite + forsterite + vapor = monticellite + liquid calcite + monticellite + forsterite + vapor = åkermanite + liquid. The eutectic liquid has high MgO/CaO and CO2/H2O and only 2–3% SiO2 (estimated 15–20% MgCO3, 35–40% CaCO3, 40–45% Mg(OH)2, and 5–6% Mg2SiO4). The composition joins intersect a thermal maximum for åkermanite + forsterite + vapor = liquid, which separates high-temperature liquids precipitating silicates together with a little calcite, from low-temperature liquids precipitating carbonates with a few percent of forsterite; there is no direct path between the silicate and synthetic carbonatite liquids on these joins, but it is possible that fractionating liquid paths diverging from the joins may connect them. More complex relationships involving the pprecipitatioon off monticellite and åkermanite are also outlined. Magnetite-magnesioferrite may replace periclase in natural magmatic systems. The results indicate that the assemblage calcite-dolomite-magnetite-forsterite represents the closing stages of crystallization of carbonatites, whereas assemblages such as calcite-magnetite-forsterite and dolomite-magnetite-forsterite span the whole range of carbonatite evolution in terms of temperature and composition, and provide the link between liquids precipitating silicates and those precipitating carbonates.
Die Beziehungen zwischen silikarischen Schmelzen und karbonatbildenden Schmelzen im System CaO-MgO-SiO2-CO2-H2O bei 2 kbar
Zusammenfassung Phasenfelder, die durch den Schnitt von drei Verbindungslinien im System CaO-MgO-SiO2-CO2-H2Odefiniert werden, wurden experimentell bei 2 kbar untersucht, um die Schmelzbeziehungen und die Kristallisationsfolge von Schmelzen, die gleichzeitig silikatische und karbonatische Minerale ausscheiden, zu bestimmen. Diese Linien verbinden SiO2 mit drei Mischungen von CaCO3-M9CO3-Mg(OH)2 mit Zusammensetzungen im primären Calcitfeld, zwischen der Zusammensetzung CaCO3 und der tieftemperierten (650°C Calcit-, Dolomit- und Periklasbildenden eutektischen Schmelze. Zwei wichtige im ppseudo-quaternären Tetraeder Calcit-Magnetit-Brucit-Diopsid gefundene Reaktionen sind: (1) Ein Eutektikum bei 650°C Calcit + Dolomit + Periklas + Forsterit + Vapor = Liquid und (2) ein Peritektikum bei 1038°C mit entweder Calcit + Åkermanit + Forsterit + Vapor = Monticellit + Liquid oder Calcit + Monticellit + Forsterit + Vapo = Åkermanit + Liquid Die eutektische Schmelze zeigt hohe MgO/CaO und CCO2H2O Verhältnisse und nur 2–3% SiO2(geschätzter Anteil an MgCO315–20%, CaCO3 35–40%, Mg(OH)2 40–50% und Mg2SiO4 5–6%). Die Verbindungslinie schneidet ein thermisches Maximum von Åkermanit + Forsterit + Vapor = Liquid, das höher temperierte Schmelzen, die Silikate gemeinsam mit etwas Clacit ausscheiden, von tiefer temperierten Schmelzen trennt, aus denen sich Karbonate gemeinsam mit wenigen Prozenten Forsterit abscheiden. Es existiert keine direkte Verbindung zwischen silikatischen und synthetischen karbonatitischen Schmelzen entlang dieser Verbindungslinien, es wäre aber möglich, daß Fraktionierungspfade, die von diesen Verbindungslinien ausgehen, sie verbinden. Komplexere Beziehungen, die die Kristallisation von Monticellit und Åkermanit beinhalten, werden ebenfalls aufgezeigt. Magnetit-Magnesioferrit könntean die Stelle von Periklas in nnatürlichenmagmatischen Systemen treten. Die Ergebnisse weisen darauf bin, daß die Vergesellschaftung Calcit-Dolomit-Magnetit-Forsterit das Endstadium der Karbonatitkristallisation repräsentiert, während die Vergesellsschaftungen von Calcit-Magnetit-Forsterit bzw. Dolomit-Magnetit-Forsterit die gesamte Spannweite der Karbonatitevolution hinsichtlich Temperatur und Zusammensetzung umfassen und demnach ein Verbindungsglied zwischen silikat- und karbonatausscheidenden Schmelzen darstellen.

With 8 Figures  相似文献   

18.
Variations in bulk Mg/Si ratios in the various groups of chondritic meteorites indicate that Mg/Si fractionation occurred in the primitive solar nebula. Enstatite (MgSiO3) evaporates incongruently forming forsterite (Mg2SiO4) as an evaporation residue; therefore, evaporation of enstatite produces Mg/Si variations in solid (Mg-rich) and gas (Si-rich) and must be considered as a probable process responsible for Mg/Si fractionation recorded in chondrites. To understand the evaporation kinetics of enstatite, incongruent evaporation experiments on enstatite single crystals have been carried out in vacuum and in hydrogen gas at temperatures of 1300 to 1500°C. A polycrystalline forsterite layer is formed on the surface of enstatite by preferential evaporation of the SiO2 component, both in vacuum and in hydrogen gas. The thickness of the forsterite layer in vacuum increases with time in the early stage of evaporation and later the thickness of the forsterite layer remains constant (several microns). This is due to the change in the rate limiting process from surface reaction plus nucleation and growth to diffusion in the surface forsterite layer. The activation energy of the diffusion-controlled evaporation rate constant of enstatite is 457 (±58) kJ/mol. A thinner forsterite layer is formed on the surface of enstatite in hydrogen gas than in vacuum. Evaporation of enstatite in hydrogen gas is also considered to be controlled by diffusion of ions through the forsterite layer. The thin forsterite layer formed in hydrogen gas is ascribed to the enhanced evaporation rate of forsterite in the presence of hydrogen gas.The results are applied to incongruent evaporation under the solar nebular conditions. The steady thickness of the forsterite of nebular pressure-temperature conditions is estimated to be submicron because of the enhanced evaporation rate of forsterite under hydrogen-rich nebular conditions if evaporated gases are taken away immediately and no back reaction occurs (an open system). Because enstatite grains in the solar nebula would be comparable to the estimated steady thickness of forsterite, evaporation of such enstatite grains under kinetic conditions could play an important role in producing variations in Mg/Si ratios between solid and gas in the solar nebula.  相似文献   

19.
Based on the in situ and temperature-quench X-ray measurements, the back transformation in the (Mg, Fe)2SiO4-spinels has been characterized in terms of the transformation temperature (T r ),mechanism and kinetics of the transformation, and of the end product(s), with specific emphasis on the effect of oxygen on this transformation. The in situ measurements were conducted to 900° C in vacuum (10-4 to 10-5 torr) and to 600° C in air using synchrotron radiation (SR) at Stanford Synchrotron Radiation Laboratory (SSRL). In the quench-type measurements, samples were heated in air to 1100° C, quenched and examined at ambient conditions using the conventional X-ray diffraction facilities. Important results are (1) in vacuum, all the spinels convert back into the olivine phase, with their T r decreasing with increasing iron content; (2) the spinel olivine back transformation is a nucleation and growth type of transformation and can be described quantitatively using the Avrami equation; (3) in air, the (Mg, Fe)2SiO4-spinels with 0.2 mole fraction Fe or more are all oxidized, and the composition and phase of the end products depend upon the temperature and the starting composition; and (4) the oxidation of the iron-rich (Mg, Fe)2SiO4-spinels in air occurs at 350–400° C, which is significantly lower than its T r ( 300° C) in vacuum.  相似文献   

20.
Stable oxygen and carbon isotopefractionation during the experimental formation ofordered norsethite (BaMg[CO3]2) from thereaction of anhydrous BaCO3 (witherite) withrelatively low concentrated sodium-magnesiumbicarbonate solutions has been studied between20° and 135 °C. In the investigatedtemperature range, 18O and 13C are enrichedin norsethite with respect to water and gaseous carbondioxide, respectively. Whereas 18O/16Opartitioning is intermediate between those of theBaCO3–H2O and MgCO3–H2O systems,13C/12C partitioning is more similar to thatfor BaCO3–CO2. Between 20° and90°C, the temperature dependences of the18O/16O and 13C/12C fractionationfactors are represented by the equations (T in °K):103 ln BaMg[CO3]2-H2O = 2.83 106T--2.85, and 103lnBaMg[CO3]2-CO2(gas) = 1.78 106T--10.16. The later equation considers carbon isotope fractionationbetween the dissolved carbonate ion and carbon dioxide measured by Halaset al. (1997). Under standard state conditions (25 °C) the fractionation factors in the system BaMg[CO3]2-CO2-H2O are: Oxygen isotopes: BaMg(CO3)2-H2O = 1.02941, BaMg(CO3)2-OH-(aq) = 1.07059,BaMg(CO3)2-CO2(gas) = 0.98868, andBaMg(CO3)2-H2CO3 * = 0.98843; carbon isotopes:BaMg(CO3)2-CO2(gas) = 1.00992,BaMg(CO3)2-H2CO3 * = 1.01099,BaMg(CO3)2-HCO3 - = 1.00194,BaMg(CO3)2-CO3 2- = 1.00491 or 1.00150.The spontaneous precipitation of aBaMg[CO3]2 gel at 20 °C,followed by the alteration of the products at20° or 60°C for 31 days,demonstrated isotope exchange reactions betweensolids and mother solutions dueto recrystallization. Isotope equilibrium, wasnot reached within run time.  相似文献   

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