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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
NASA NTRS2007

Oxidation State of Nakhlites as inferred from Fe-Ti oxide Equilibria and Augite/Melt Europium Partitioning

Recent studies have shown that Martian magmas had wide range of oxygen fugacities (fO2) and that this variation is correlated with the variation of La/Yb ratio and isotopic characteristics of the Martian basalts, shergottite meteorites. The origin of this correlation must have important information about mantle sources and Martian evolution. In order to understand this correlation, it is necessary to know accurate value of oxidation state of other Martian meteorite groups. Nakhlites, cumulate clinopyroxenites, are another major group of Martian meteorites and have distinctly different trace element and isotopic characteristics from shergottites. Thus, estimates of oxidation state of nakhlites will give us important insight into the mantle source in general. Several workers have estimated oxidation state of nakhlites by using Fe-Ti oxide equilibrium. However, Fe-Ti oxides may not record the oxidation state of the parent melt of the nakhlite because it is a late-stage mineral. Furthermore, there is no comprehensive study which analyzed all nakhlite samples at the same time. Therefore, in this study (1) we reduced the uncertainty of the estimate using the same electron microprobe and the same standards under the same condition for Fe-Ti oxide in 6 nakhlites and (2) we also performed crystallization experiments to measure partition coefficients of Eu into pyroxene in the nakhlite system in order to estimate fO2 when the pyroxene core formed (i.e. Eu oxybarometer [e.g. 2,6]).

Makishima, J.↗
DOE OSTI2023

Plutonium Signatures in Molten-Salt Reactor Off-Gas Tank and Safeguards Considerations

Fluid-fueled molten-salt reactors (MSRs) are actively being developed by several companies, with plans to deploy them internationally. The current IAEA inspection tools are largely incompatible with the unique design features of liquid fuel MSRs (e.g., the complex fuel chemistry, circulating fuel inventory, bulk accountancy, and high radiation environment). For these reasons, safeguards for MSRs are seen as challenging and require the development of new techniques. This paper proposes one such technique through the observation of the reactor’s off-gas. Any reactor design using low-enriched uranium will build up plutonium as the fuel undergoes burnup. Plutonium has different fission product yields than uranium. Therefore, a shift in fission product production is expected with fuel evolution. The passive removal of certain gaseous fission products to the off-gas tank of an MSR provides a valuable opportunity for analysis without significant modifications to the design of the system. Uniquely, due to the gaseous nature of the isotopes, beta particle emissions are available for observation. The ratios of these fission product isotopes can, thus, be traced back to the relative amount and types of fissile isotopes in the core. This proposed technique represents an effective safeguards tool for bulk accountancy which, while avoiding being onerous, could be used in concert with other techniques to meet the IAEA’s timeliness goals for the detection of a diversion.

Dunkle, Nicholas (ORCID:000000027323011X)↗
NASA NTRS1989

The evolution of complex type B Allende inclusion - An ion microprobe trace element study

Results are presented of a detailed trace-element and isotopic analyses of the constituent phases in each of the major textural parts (mantle, core, and islands) of a Type B refractory inclusion, the USNM 5241 inclusion from Allende, first described by El Goresy et al. (1985). The REE data on 5241 were found to be largely consistent with a model in which the mantle and the core of 5241 formed sequentially out of a single melt by fractional crystallization. The numerical models of REE evolution in the 5241 melt, especially that of Eu, require that a significant mass of spinel-free island material was assimilated into the evolving melt during the last half of the solidification history of 5241. The trace element results pbtained thus strongly support the interpretation of El Goresy et al. (1985) that the spinel-free islands in the 5241 are trapped xenoliths.

Macpherson, Glenn J.↗
NASA NTRS2014

Preliminary Report on U-Th-Pb Isotope Systematics of the Olivine-Phyric Shergottite Tissint

Geochemical studies of shergottites suggest that their parental magmas reflect mixtures between at least two distinct geochemical source reservoirs, producing correlations between radiogenic isotope compositions, and trace element abundances.. These correlations have been interpreted as indicating the presence of a reduced, incompatible-element- depleted reservoir and an oxidized, incompatible-element-rich reservoir. The former is clearly a depleted mantle source, but there has been a long debate regarding the origin of the enriched reservoir. Two contrasting models have been proposed regarding the location and mixing process of the two geochemical source reservoirs: (1) assimilation of oxidized crust by mantle derived, reduced magmas, or (2) mixing of two distinct mantle reservoirs during melting. The former clearly requires the ancient martian crust to be the enriched source (crustal assimilation), whereas the latter requires a long-lived enriched mantle domain that probably originated from residual melts formed during solidification of a magma ocean (heterogeneous mantle model). This study conducts Pb isotope and U-Th-Pb concentration analyses of the olivine-phyric shergottite Tissint because U-Th-Pb isotope systematics have been intensively used as a powerful radiogenic tracer to characterize old crust/sediment components in mantle- derived, terrestrial oceanic island basalts. The U-Th-Pb analyses are applied to sequential acid leaching fractions obtained from Tissint whole-rock powder in order to search for Pb isotopic source components in Tissint magma. Here we report preliminary results of the U-Th-Pb analyses of acid leachates and a residue, and propose the possibility that Tissint would have experienced minor assimilation of old martian crust.

Moriwaki, R.↗
NASA NTRS2018

A Complex History of Silicate Differentiation of Mars from Nd and Hf Isotopes in Crustal Breccia NWA 7034

Resolving the possible mantle and crustal sources for shergottite meteorites is crucial for understanding the formation and early differentiation of Mars. Orbiter and rover characterization of the martian surface reveal that the major element composition of most of its surface does not match the shergottites (McSween et al., 2009)leaving the relationship between them poorly understood. The identification of the meteorite NWA 7034 and its pairs as a Mars surface rock (Cartwright et al., 2014)provides access to a representative sample of Mars' crust (Agee et al., 2013;Humayun et al., 2013). Utilizing the short-lived Sm-146 - Nd-142, and long-lived Sm-142 - Nd-142 and Lu-176 - Hf-176 chronometers, which are sensitive to silicate differentiation, we analyzed three fragments of NWA 7034. The very negative mean isotopic compositions for this breccia, μNd-142(sub JNdi-1)=−45 +/-5(2SD), εNd-143(sub CHUR)=−16.7 +/-0.4(2SD) and εHf176(sub CHUR)=−61 +/-9(2SD) point to an ancient origin for this martian crust. However, modeling of the data shows that the crust sampled by NWA 7034 possesses a Hf/Nd ratio and coupled εNd-143 - μNd-142 model age that are incompatible with this crustal reservoir being an end-member that generated the shergottite source mixing array. In addition, this crust is not juvenile, despite its rare earth element profile, but has had a multistage formation history. Therefore, early crustal extraction alone was not responsible for the creation of the reservoirs that produced the shergottites. Instead mantle reservoirs formed via other early differentiation processes such as in a Mars magma ocean must be responsible for the trace element and isotopic signatures present in shergottites.

Rosalind M. G. Armytage↗
DOE OSTI2021

Volatile Element Evidence of Local MORB Mantle Heterogeneity Beneath the Southwest Indian Ridge, 48°–51°E

Abstract The mantle source beneath the Southwest Indian Ridge (SWIR) reflects a complex history of contamination. Magmatic volatile contents are vital tracers of these kinds of heterogeneities, which may fractionate otherwise constant volatile/non‐volatile elemental ratios, such as the H 2 O/Ce ratio. Although several studies have recently used trace element and isotopic data to address mantle source heterogeneity and magmatic processes at SWIR 48°–51°E region, volatile element constraints provide a valuable test of models for the origins of mantle heterogeneities in this region. Here, we present new data for nine rare basaltic glass samples from the 48°–51°E region, which enable careful assessment of the effects of primary versus secondary processes on the glass volatile contents. These samples are strongly affected by variable extents of carbon degassing, and shallow assimilation of Cl‐rich fluid, but also reveal consistently high H 2 O/Ce ratios (458.8 ± 14.9), among the highest in MORBs, that cannot be explained by late‐stage secondary processes, crustal assimilation, or simple melting of peridotite mantle at variable depths. Instead, the high H 2 O/Ce ratios are features of the mantle source composition. The 48°–51°E region is notably more depleted in highly incompatible trace elements relative to other regions of the SWIR, although this depletion is not apparent in H 2 O, which is similarly abundant throughout the SWIR. We link the high H 2 O/Ce ratios in these glasses with other trace element characteristics diagnostic of subduction and fluid addition, suggesting that the mantle source reflects signatures of a refractory mantle residue that previously melted within a subduction zone.

Wang, Wei↗
NASA NTRS2014

A FIB/TEM/Nanosims Study of a Wark-Lovering Rim on an Allende CAI

Ca- Al-rich inclusions (CAIs) are commonly surrounded by Wark-Lovering (WL) rims - thin (approx. 50 micrometers) multilayered sequences - whose mineralogy is dominated by high temperature minerals similar to those that occur in the cores of CAIs [1]. The origins of these WL rims involved high temperature events in the early nebula such as condensation, flashheating or reaction with a nebular reservoir, or combinations of these processes. These rims formed after CAI formation but prior to accretion into their parent bodies. We have undertaken a coordinated mineralogical and isotopic study of WL rims to determine the formation conditions of the individual layers and to constrain the isotopic reservoirs they interacted with during their history. We focus here on the spinel layer, the first-formed highest- temperature layer in the WL rim sequence. Results and Discussion: We have performed mineralogical, chemical and isotopic analyses of an unusual ultrarefractory inclusion from the Allende CV3 chondrite (SHAL) consisting of an approx. 500 micrometers long single crystal of hibonite and co-existing coarsegrained perovskite. SHAL is partially surrounded by WL rim. We previously reported on the mineralogy, isotopic compositions and trace elements in SHAL [2-4]. The spinel layer in the WL rim is present only on the hibonite and terminates abruptly at the contact with the coarse perovskite. This simple observation shows that the spinel layer is not a condensate in this case (otherwise spinel would have condensed on the perovskite as well). The spinel layer appears to have formed by gas-phase corrosion of the hibonite by Mg-rich vapors such that the spinel layer grew at the expense of the hibonite. We also found that the spinel layer has the same 16Orich composition as the hibonite. The spinel layer is polycrystalline and individual crystals do not show a crystallographic relationship with the hibonite. An Al-diopside layer overlies the spinel layer, and is present on both the hibonite and perovskite. While the spinel is 16O-rich, WL-rim perovskite and pyroxene are 16O-poor. This isotopic heterogeneity likely reflects O isotopic equilibration of WL-rim perovskite and pyroxene with a planetary O isotopic reservoir after the WL rim formation. The hibonite is zoned and contains wt.% levels of Ti, Mg and Fe in contact with the Fe-bearing spinel (Sp60Hc40) in the WL rim. The Fe enrichment in spinel is likely related to the Na-Fe metasomatism that is ubiquitous in Allende. Conclusions: The petrography and microstructure of the spinel layer in a WL rim sequence shows that it formed by gas phase reactions at high temperature in the nebula. The oxygen isotopic composition of the spinel indicates that this WL rim layer formed in the same (or similar) nebular gas reservoir as the host CAI.

Keller, L. P.↗
DOE OSTI2022

Resonance ionization of zirconium

Abstract Measuring the isotopic composition of trace Zr in presolar stardust grains allows us to study the environment of slow neutron-capture nucleosynthesis in asymptotic giant branch stars. Here, we present a newly characterized Zr resonance ionization scheme that can be saturated with state-of-the-art titanium-sapphire lasers and yields a useful yield of (5.4 ± 0.4)%. Resonance ionization is achieved in two steps: after first being excited with a photon at 319.215 nm, neutral Zr atoms are then ionized with a photon at 388.988 nm, where both wavelengths are reported as in vacuum.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Iron precipitation under controlled oxygen flow: Mineralogical implications for BIF precursors in the Archean ocean

Banded iron formation (BIF) deposition in the Archean ocean is thought to have been initiated by the oxidation of dissolved iron into ferric primary precursor phases that descended through the water column and were deposited on the seafloor. Effective interpretation of the trace element and isotopic composition of BIFs in the geologic record requires an understanding of the identity and longevity of those precursor phases. Temporal and spatial variation in oxidant concentration and ocean chemistry may have driven precursor mineralogy. Furthermore, precursor phases may undergo transitions during descent and burial. This experimental study follows the evolution of iron mineralogy, speciation, and redox state during the precipitation of iron under variable oxygen fluxes and in fluids containing different iron-complexing anions (chloride, sulfate, and phosphate). Additionally, suspensions collected after incomplete oxidation were anoxically aged to simulate changes to precursor mineralogy during descent below the seawater redoxcline. Results from X-ray diffraction, sequential dissolution, colorimetric determination of Fe redox state, and Fe K-edge X-ray absorption fine structure spectroscopy showed that under all experimental conditions, intermediate precipitates collected before complete iron uptake contained mineralized ferrous iron. Purely ferric mineral assemblages were not observed until iron was removed from solution. In low-oxygen experiments, intermediate precipitates contained phases with stoichiometric Fe 2+ , including magnetite, vivianite, and green rust (GR). Chloride green rust (GR1) had more ferric iron than sulfate green rust (GR2) and more readily transitioned to magnetite via disproportionation. GR2 was stable over a broader range of iron uptake; magnetite appeared mainly as an additional oxidation product in sulfate solution. In high oxygen experiments, mineralized ferrous iron occurred in amorphous phases or as a non-stoichiometric component in ferric oxides; final ferric assemblages were less crystalline than in low-oxygen equivalents. Low concentrations of phosphate increased the total iron oxidation rate, but also increased the ferrous content of intermediate precipitates. The incorporation of phosphate stabilized GR2 and facilitated GR2 precipitation over a larger range of iron uptake. In higher concentrations of phosphate, vivianite and poorly crystalline ferric hydroxides formed in place of GR. Here, these findings suggest that over a range of possible ocean chemistries, mixed-valence phases may have been short lived but relevant precursors to BIF. Additionally, anionic chemistry and oxidant concentration are shown to influence the crystallinity and chemical resistivity of final ferric assemblages, affecting their reactivity during later anoxic burial.

58 GEOSCIENCES↗
DOE OSTI2021

Changing chemistry of particulate manganese in the near- and far-field hydrothermal plumes from 15°S East Pacific Rise and its influence on metal scavenging

Dissolved Mn(II) in the hydrothermal plume is known to be microbially oxidized to form Mn(III/IV) oxides, and the Mn oxides scavenge other trace elements in seawater. In the GEOTRACES GP16 cruise, dissolved Mn (dMn) and particulate Mn (pMn) were found to be transported over 4000 km westwards from the Southern Eastern Pacific Rise. Previous studies in this plume showed different removal rates of dMn and pMn as well as pMn size distribution between the near-field (<80 km from the ridge axis) and far-field (>80 km) plumes. In order to understand Mn cycling in these plumes, spatial distribution, oxidation states, and mineral structures of Mn in small size fraction (SSF; 0.8–51 μm) and large size fraction (LSF; >51 μm) particles from the near-field and far-field plumes were examined using micro X-ray fluorescence spectrometry (μ-XRF), X-ray absorption near-edge structure spectroscopy (XANES), chemical species mapping, and extended X-ray absorption fine-structure spectroscopy (EXAFS). In the near-field plume, pMn in the SSF is dominated by oxidized Mn with Mn(III) fractions of ~30%. They are a mixture of δ-MnO 2 and triclinic birnessites that is known to be formed as a result of autocatalytic Mn(II) oxidation at the surface of freshly-formed δ-MnO2, suggesting that both microbial and autocatalytic Mn oxidation occur in the near-field plume. The LSF pMn in the near-field plume is also oxidized and often found in large aggregates several hundreds of μm in size. These aggregates settle out in the near-field and during transport, and are not found in the far-field plume. In the far-field plume where Mn oxides are not newly formed, pMn in the SSF is oxidized, but their Mn(III) fractions are smaller than in the near-field pMn. Unlike the SSF, the far-field plume LSF pMn is dominated by reduced Mn, implying very slow aggregation of pMn in the far-field plume. The different characteristics of pMn between the near-field and far-field plumes affect its scavenging of other trace elements. In the near-field plume, Co, Mo, 231 Pa are associated with pMn, but not in the far-field plume. 231 Pa is adsorbed to pFe rather than pMn in the far-field plume, and Pb is adsorbed to pFe in the entire plume. The result shows that freshly-formed Mn oxides in the near-field plume have higher scavenging capacity than the far-field plume pMn. Our findings suggest that the mineralogical age of Mn oxides may be an important parameter that controls the scavenging of many other trace elements and isotopes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Galaxy Serpent V - Answers to second inject

Based on the U isotopic compositions and trace element concentrations - additional information provided in Inject 1b - we assess that the two samples are inconsistent with high confidence. Our assessment factored in the results of the graded decision framework (GDF) as well as expert knowledge of these kind of measurements.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
NASA NTRS1977

The supernova trigger for formation of the solar system

It is suggested that the explosion of a Type II supernova triggered the collapse of a nearby interstellar cloud and led to the formation of the solar system. Estimates of the abundances resulting from nuclear processing of the supernova ejecta are presented. It appears promising that nucleosynthesis in this single supernova event can account for most isotopic anomalies and traces of extinct radioactivities in solar-system material.

Cameron, A. G. W.↗
NASA NTRS1977

Chemistry of Apollo 12 mare basalts - Magma types and fractionation processes

Major and trace element data for a large suite of petrographically diverse Apollo 12 mare basalts are presented, and magma types sampled at the Apollo 12 site are characterized. The data confirm earlier classifications of the basalts into olivine, pigeonite, ilmenite, and feldspathic basalts. The olivine and pigeonite basalts are shown to be comagnetic and related by olivine fractionation. The other types, which differ in trace element and isotopic characteristics, are derived from different sources within the lunar interior. The spatial relations between the main basalt types are discussed in terms of local cratering events, and it is suggested that the younger ilmenite basalts overlie the olivine-pigeonite basalts. The role of olivine-dominated near-surface crystal fractionation in causing chemical variation is examined, and a relation between inferred cooling rate and the position of a sample in the fractionation sequence is determined.

Rhodes, J. M.↗
NASA NTRS1982

Age and provenance of the target materials for tektites and possible impactites as inferred from Sm-Nd and Rb-Sr systematics

Chemical, trace element, and isotopic compositions of tektites are consistent with production by melting of sediments derived from the old terrestrial continental crust. Each tektite group is characterized by a uniform Nd model age, interpreted as the time of formation of the crustal segment which weathered to form the parent sediment for the tektites. Sr model ages are variable within each group, reflecting Rb-Sr fractionation, and, in the favorable limit of very high Rb/Sr ratios, approach the time of sedimentation of the parent material which melted to form the tektites. Unlike tektites, which are dense homogeneous objects, sanidine spherules are porous, fine grained inhomogeneous objects. The leaching experiment employed by the present study shows that the sanidine spherules could have been formed by an oceanic impact involving basaltic crust and overlying sediments or seawater.

Shaw, H. F.↗
NASA NTRS1985

Lunar and Planetary Science Conference, 16th, Houston, TX, March 11-15, 1985, Proceedings. Part 1

Various papers on lunar studies, meteorites and cosmic dust, Mars, and tektites are presented. The topics discussed include: very high potassium basalt; complications in mare basalt petrogenesis; mare basalt genesis; modeling trace elements and isotopic ratios; Zr-Hf-Ta fractionation during lunar evolution; petrology of the Apollo 12 highland component; petrologic province maps of the lunar highlands derived from orbital geochemical data; petrology and chemistry of Apollo 12 regolith breccias; chemical variability and origin of agglutinitic glass; multistage exposure history of the 74261 soil constituents; and an experimental investigation of agglutinate melting mechanisms; shocked mixtures of sodium and potassium feldspars. Also addressed are: cooling history of some Antarctic ureilites; the Leoville accretionary breccia; ubiquitous brecciation after metamorphism in equilibrated ordinary chondrites; layer silicates in a chondritic porous interplanetary dust particle; estimates of rheological properties for flows on the Martian volcano Ascraeus Mons; the Martian dust storm of Sol 1742; and late Eocene North American microtektites and clinopyroxene-bearing spherules.

Ryder, G.↗
NASA NTRS1988

Murchison xenoliths

C3 xenoliths in a C2 host (Murchison) are unique among known meteoritic xenolith-host occurrences. They offer an opportunity to determine possible effects on the xenoliths by the hydrated host. Eleven xenoliths were found ranging from 2 to 13 mm. Four of these Murchison Xenoliths (MX1, MX2, MX3 and MX4) have been studied in detail. MX1 and MX2 were large enough for trace element, oxygen isotope, carbon isotope, bulk carbon and bulk nitrogen determinations. All four were studied petrographically and by analytical SEM. The xenoliths cannot be unequivocally identified as C3V or C3O subtypes. MX1 contains some matrix phyllosilicate, indicating reaction with water. MX1, MX2 and MX3 all show extensive alteration by an FeO-rich medium, and some minerals in them contain ferric iron. MX4, however, exhibits very minor alteration by FeO only. Oxygen isotopic and chemical data show that the alteration of these xenoliths did not take place in the Murchison host. The alterations occurred in one or more parent bodies, which were later disrupted to release these xenoliths that ultimately accreted onto the Murchison parent body.

Olsen, Edward J.↗
NASA NTRS1988

Geochemical comparison of K-T boundaries from the Northern and Southern Hemispheres

Closely spaced (cm-scale) traverses through the K-T boundary at Stevns Klint (Denmark), Woodside Creek (New Zealand) and a new Southern Hemisphere site at Richards Bay (South Africa) were subjected to trace element and isotopic (C, O, Sr) investigation. Intercomparison between these data-sets, and correlation with the broad K-T database available in the literature, indicate that the chemistry of the boundary clays is not globally constant. Variations are more common than similarities, both of absolute concentrations, and interelement ratios. For example, the chondrite normalized platinum-group elements (PGE) patterns of Stevns Klint are not like those of Woodside Creek, with the Pt/Os ratios showing the biggest variation. These differences in PGE patterns are difficult to explain by secondary alteration of a layer that was originally chemically homogeneous, especially for elements of such dubious crustal mobility as Os and Ir. The data also show that enhanced PGE concentrations, with similar trends to those of the boundary layers, occur in the Cretaceous sediments below the actual boundary at Stevns Klint and all three the New Zealand localities. This confirms the observations of others that the geochemistry of the boundary layers apparently does not record a unique component. It is suggested that terrestrial processes, eg. an extended period of Late Cretaceous volcanism can offer a satisfactory explanation for the features of the K-T geochemical anomaly. Such models would probably be more consistent with the observed stepwise, or gradual, palaeontological changes across this boundary, than the instant catastrophe predicated by the impact theory.

Tredous, M.↗
NASA NTRS1989

Viking and Mars Rover exobiology

Other than Earth, Mars is the planet generating the greatest interest among those researching and contemplating the origin and distribution of life throughout the universe. The similarity of the early environments of Earth and Mars, and the biological evolution on early Earth provides the motivation to seriously consider the possibility of a primordial Martian biosphere. In 1975 the Viking project launched two unmanned spacecraft to Mars with the intent of finding evidence of the existence of present or past life on this planet. Three Viking Biology experiments were employed: the Labeled Release experiment, the Gas Exchange Experiment, and the Pyrolytic Release experiment. Each of these three experiments tested for microbial existence and utilization of a substrate by examining the gases evolved from specific chemical reactions. Although the results of these experiments were inconclusive, they inferred that there are no traces of extant life on Mars. However, the experiments did not specifically look for indication of extinct life. Therefore, most of the exobiologic strategies and experiments suggested for the Mars Rover Sample Return Mission involve searching for signature of extinct life. The most significant biological signatures and chemical traces to detect include: isotopic and chemical signatures of metabolic activity, anomalous concentrations of certain metals, trace and microfossils, organically preserved materials, carbonates, nitrates, and evaporites.

Schwartz, D. E.↗