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All sourcesNASA NTRSDOE OSTI
NASA NTRS2020

Ag isotopic and chalcophile element evolution of the terrestrial and martian mantles during accretion: new constraints from Bi, Pd, and Ag metal-silicate partitioning.

The Earth’s timing of accretion and acquisition of moderately volatile compounds is uncertain. Hafnium-W and Mn-Cr isotopic data can bracket the timing of early planetary differentiation and core formation. The Ag-Pd system has also been utilized but its application has been limited by a lack of high pressure and temperature metal-silicate partitioning for Pd and Ag. Be-cause Ag (and Bi) are volatile chalcophile siderophile elements, understanding their early distribution can constrain the origin of volatile elements in differentiated bodies and planets. Unfortunately, neither Ag or Bi have been studied across the wide range of pressure and temperature conditions that are relevant to accretion and core-mantle differentiation. Here, new high-pressure and temperature multi-anvil metal-silicate equilibrium experiments for Bi and Ag have been carried out at conditions relevant to planetary accretion and metal silicate differentiation that allow a more refined and complete understanding of element partitioning during core formation. The new metal-silicate partitioning data utilized to predict the distributions of Bi, Pd, and Ag at conditions of accretion for Earth and Mars and show that the Pd/Ag ratio is significantly fractionated during accretion, allowing for the production of detectable 107Ag anomalies produced while 107Pd (half life = 6.5 M.y.) was still extant. Application of the new partitioning results to Earth shows that D(Bi) and D(Ag) (D = metal/silicate concentration ratio) are lowered due to the effect of pressure and Si alloyed in the metallic liquid, resulting in higher predicted mantle Bi and Ag abundances than in the bulk silicate Earth (BSE), as well as high and variable Pd/Ag. The unradiogenic Ag isotopic composition of the BSE could have been generated by early accretion of volatile-poor (high Pd/Ag) precursors, followed by later accretion of volatile–rich (low Pd/Ag) material, in agreement with earlier studies of Pd-Ag and Mn-Cr (Schönbächler et al., 2010). However, these main accretion phases would have to be followed by segregation of a sulfide liquid (at least 1.5% of magma ocean) at high pressures (>30 GPa), to explain the PUM Bi, Pd, and Ag, as well as Au, Pt, Cu and Ni concentrations as proposed previously. If the early accreted bulk Earth was volatile depleted with high Pd/Ag ratios, portions of the mantle may contain ancient domains that developed positive 107Ag isotopic anomalies (as also argued by noble gases, Nd, W, and Os isotopes). In comparison, Bi, Pd, and Ag concentrations in the martian mantle could have been set by simple metal-silicate equilibrium. Mars accreted and differentiated relatively rapidly, while also developing a deep magma ocean with a high Pd/Ag ratio that could have evolved positive 107Ag anomalies, in contrast to Earth. Measurements on shergottites may reveal these predicted Ag isotopic anomalies.

accretion↗
NASA NTRS2020

A Multi-Sims Investigation of Water Content and D/H Ratios in Roberts Massif 04262 with Insight to Sources of Hydrogen in Maskelynite

We want to define the H2O content ([H2O]) and hydrogen (H) isotope composition of meteoritic material from Mars [1-3] with motivation to understand Mars’ volatile history, constrain geochemical signatures of interior water reservoirs (i.e. the Martian mantle) and explore effects of planetary (e.g. planet formation, magma ocean degassing) and local (e.g. volcanic degassing, impact melting and degassing) processes on H incorporated in minerals. Secondary ion mass spectrometry (SIMS) allows multiple avenues to address these questions. However, application to (1) precious astromaterials and (2) low level H measurements, pose specific challenges that are further complicated when combined. We present preliminary data of a multi-approach (SIMS vs. NanoSIMS) study of H in Roberts Massif 04262 (RBT 04262), an enriched lherzolitic shergottite with nonpoikilitic (NP) and poikilitic (P) lithologies [4]. We analyze olivine, pyrox-ene, and melt inclusions to compare indigenous mantle water, with impact-generated maskelynite to investigate H signatures due to shock.

Dudley, J. M.↗
DOE OSTI2026

Role of Surface Hydroxyls and Lattice Oxygen in Governing Selectivity and Restructuring During Acetic Acid Conversion on Fe 3 O 4 (001)

Understanding the reactivity of carboxylic acids on metal oxide surfaces is critical for elucidating ketonization mechanisms relevant to biomass upgrading. Here, we investigate the adsorption and thermal decomposition of acetic acid (CH 3 COOH) on Fe 3 O 4 (001) using scanning tunneling microscopy (STM), temperature-programmed reaction spectroscopy (TPRS), and X-ray photoelectron spectroscopy (XPS). At room temperature, acetic acid adsorbs dissociatively to form ordered bidentate acetate (CH 3 COO) overlayer that lifts the (√2 × √2)R 45° surface reconstruction. TPRS reveals ketene (CH 2 CO) as the dominant product, along with CO, CO 2 , and H 2 O, the latter evolving via a Mars–van Krevelen (MvK) mechanism. Isotopic labeling shows preferential CO 2 formation from the carboxyl carbon and a more balanced CO/CO 2 ratio from the methyl carbon, suggesting distinct oxidation pathways. STM imaging reveals embedded acetate intermediates filling surface oxygen vacancies created in MvK steps. Upon product formation completion (~700 K), extensive surface etching is observed, with pits elongated along the octahedral Fe rows. Approximately 20% of the surface oxygen is removed, consistent with vacancy formation stoichiometry inferred from product distributions. These findings demonstrate that carboxylate-induced restructuring of Fe 3 O 4 (001) involves both surface healing and reduction processes, offering mechanistic insights relevant to ketonization and broader carboxylic acid chemistry on metal oxides.

acetic acid↗
NASA NTRS1980

Neutron capture time scale of the s-process, estimated from s-process krypton in a meteorite

A krypton fraction enriched in s-process isotopes was extracted from a mineral fraction of the Murchison C2 chondrite. The (Kr-86)/(Kr-84) ratio is enhanced by 6 standard deviations, showing that significant amounts of Kr-86 were made in the s-process, despite the short, 10.8 yr beta-decay half-life of its precursor, Kr-85. Judging from this sample, the mean neutron capture time in the s-process was on the order of 5-100 yr for nuclei with cross sections of 125 mb.

Matsuda, J.-I.↗
NASA NTRS2020

A new model of monodeuterated ethane (C2H5D) spectrum: Enabling sensitive constraints on the D/H in ethane emission in comets

Similar to ethane (C2H6), monodeuterated ethane (C2H5D) has a bright series of Q-branches in the CH stretch region, between about 2960 - 3020 cm (3.38 - 3.31 µm). As the progressions in the different isotopes are slightly offset from one another, the new C2H5D model enables sensitive constrains of the D/H ratio in spectra from comets, in organics across the Solar System and beyond. Specifically, the D/H ratio of organic molecules in comets is a critical cosmogenic indicator, which not only provides insights into the formation processes of our Solar System, but also allows for a test of our understanding of solid-state astrochemistry. High D/H ratios are predicted in a number of astrochemical models, which can be benchmarked using the new spectroscopic information of C2H5D and C2H6. We present a quantum band model for C2H5D in the mid-infrared. Our model is based on rotationally resolved spectra of C2H5D and C2H6 obtained at 85K between 2050 - 3050 per cm (4.88 - 3.28 µm) using a Bruker IFS-125HR equipped with a cryogenic Herriott cell at JPL. High-level quantum chemical calculations were carried out at the CCSD(T)/ANO1 level of theory to aid vibrational assignments, with the anharmonic frequencies and vibrational corrections determined from second-order vibrational perturbation theory (VPT2). As a first demonstration of the applicability of the model, we obtained a stringent upper limit to the organic D/H ratio (18.2 VSMOW) in comet C/2007 W1 (Boattini) from high resolution fluorescence spectra obtained with Keck/NIRSPEC.

Kirstin D. Doney↗
NASA NTRS1993

The case of missing CO-13 in mergers

We present a comparison of the CO-13 and CO-12 emissions of six systems of merging galaxies: NGC 828, NGC 3256, NGC 4194, NGC 6240, Arp 220, and Arp 299. The observations were made in both J=1-0 and J=2-1 transitions with the IRAM 30 m and SEST 15 m telescopes. In all galaxies but NGC 828, the CO-13 is much weaker than in spiral galaxies. The average emissivity ratios measured at the few kiloparsec scale are: CO-12(1-0)/CO-13(1-0) approx. equals 30, CO-12(2-1)/CO-13(2-1) approx. equals 40. These values are significantly larger than those usually measured in normal spiral galaxies, which are always between 5 and 15 for the J=1-0 line. We show that such a peculiar behavior cannot be interpreted as due to the dominant presence of diffuse gas and it cannot be attributed to optically thin CO emission either. The faint CO-13 emission of mergers must result from either an underabundance of CO-13 or an overabundance of CO-12. They may be accounted for by different mechanisms: CO-13 molecules are more easily photodissociated than CO-12 ones - however our observations seem to rule out physical conditions characteristic of photodissociation regions; in the course of the merging, large amounts of unprocessed gas, with a high (CO-12/CO-13) abundance ratio, are driven from the external regions of the progenitor galaxies to the new nucleus - this could increase the (CO-12/CO-13) ratio by a factor of 2; the interstellar medium can also be quickly enriched in C-12 (thus in CO-12) by a factor of 2, due to selective nucleosynthesis of this isotope (vs. C-13) in the massive stars born during the starburst. The last two processes can thus significantly contribute to the weakness of the CO-13 lines. The high CO-13-to-CO-12 line ratios that we have measured are due to the deep transformations that take place in the interstellar medium during the merging and the starburst: indeed, the only object with nearly normal line ratios, NGC 828, appears less perturbed and active in star formation than the other sources in the sample. In most mergers, the faintness of the CO-13 emission may indicate that the conversion factor from CO-12 emissivities to H2 column densities could differ substantially from the standard galactic value.

Casoli, Fabienne↗
NASA NTRS1991

A measurement of the cosmic-ray H-2 and He-3 spectra and H-2/He-4 and He-3/He-4 ratios in 1989

The energy spectra of H-2 and H-3 nuclei up to energies of 450 and 800 MeV nucleon, respectively, were measured during a balloon flight of the NASA/NMSU Balloon Borne Magnet Facility on September 5, 1989. These isotopes were cleanly resolved from the more abundant H-1 and He-4 using a measurement of rigidity versus velocity as measured in a high-resolution scintillation counter. After correction for atmospheric secondaries the measured H-2/He-4 and He-3/He-4 ratios are both consistent with the production expected if H-1 and He-4 have the same path length in the galaxy as heavier cosmic-ray nuclei such as C and Fe, to within about 20 percent. Solar modulation effects play an important role in this uncertainty. This result favors a generally similar propagation history, along with similar types of sources for H-1 and He-4 and the heavier cosmic-ray nuclei.

Webber, W. R.↗
NASA NTRS1977

Isotopic abundance of CO in interstellar clouds

The fractional abundances of the isotopic species of carbon monoxide in interstellar clouds are calculated on a basis of gas-phase ion-molecule reactions. The (C-13)O/(C-12)O ratio varies significantly with extinction of the ultraviolet radiation field, and in the outer regions of dark dense clouds (C-13)O may be enhanced by a factor of 10. The observational interpretation of the CO to H2 or interstellar-reddening relation and the isotopic abundances of carbon are complicated by these effects.

Langer, W. D.↗
DOE OSTI2021

The use of a digital micromirror array as a temporal gate and spatial-filtering device for laser-induced breakdown spectroscopy and laser ablation molecular isotopic spectrometry

A digital micromirror array (DMMA) is used in a simple and inexpensive approach for spatially resolved temporal gating of atomic emission detection in laser-induced breakdown spectroscopy (LIBS). Selected mirrors in the array are actuated at a time delayed from the primary laser pulse, permitting optical gating with a response time of 160 ns while using a conventional CCD detector. Detector gating is shown to decrease noise from short-lived spectroscopic background (both continuum and N II from air), improving signal-to-background ratios by 22-times for selected samples and emission lines. The utility of rapid temporal gating is also demonstrated for the optical detection of isotopes using the laser-ablation molecular isotope spectrometry (LAMIS) experiment. Additionally, optical temporal gating and spatial filtering are used to isolate regions of the laser-induced plasma, enhancing signal from molecular emission. The potential of the simple technique for use in field-portable LIBS and LAMIS experiments is explored.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
NASA NTRS2006

Relationships Among Intrinsic Properties of Ordinary Chondrites: Oxidation State, Bulk Chemistry, Oxygen-isotopic Composition, Petrologic Type, and Chondrule Size

The properties of ordinary chondrites (OC) reflect both nebular and asteroidal processes. OC are modeled here as having acquired nebular water, probably contained within phyllosilicates, during agglomeration. This component had high Ai70 and acted like an oxidizing agent during thermal metamorphism. The nebular origin of this component is consistent with negative correlations in H, L, and LL chondrites between oxidation state (represented by olivine Fa) and bulk concentration ratios of elements involved in the metal-silicate fractionation (e.g., NdSi, Ir/Si, Ir/Mn, Ir/Cr, Ir/Mg, Ni/Mg, As/Mg, Ga/Mg). LL chondrites acquired the greatest abundance of phyllosilicates with high (delta)O-17 among OC (and thus became the most oxidized group and the one with the heaviest O isotopes); H chondrites acquired the lowest abundance, becoming the most reduced OC group with the lightest O isotopes. Chondrule precursors may have grown larger and more ferroan with time in each OC agglomeration zone. Nebular turbulence may have controlled the sizes of chondrule precursors. H-chondrite chondrules (which are the smallest among OC) formed from the smallest precursors. In each OC region, low-FeO chondrules formed before high-FeO chondrules during repeated episodes of chondrule formation. During thermal metamorphism, phyllosilicates were dehydrated; the liberated water oxidized metallic Fe-Ni. This caused correlated changes with petrologic type including decreases in the modal abundance of metal, increases in olivine Fa and low-Ca pyroxene Fs, increases in the olivine/pyroxene ratio, and increases in the kamacite Co and Ni contents. As water (with its heavy 0 isotopes) was lost during metamorphism, inverse correlations between bulk (delta)O-18 and bulk (delta)O-17 with petrologic type were produced. The H5 chondrites that were ejected from their parent body approx.7.5 Ma ago during a major impact event probably had been within a few kilometers of each other since they accreted approx.4.5 Ga ago. There are significant differences in the olivine compositional distributions among these rocks; these reflect stochastic nebular sampling of the oxidant (Le., phyllosilicates with high (delta)O-17) on a 0.1-1 km scale during agglomeration.

Rubin, Alan E.↗
NASA NTRS2005

An Achondritic Micrometeorite from Antarctica: Expanding the Solar System Inventory of Basaltic Asteroids

Micrometeorites with sizes below 1 mm are collected in a diversity of environments such as deep-sea sediments and polar caps. Chemical, mineralogical and isotopic studies indicate that micrometeorites are closely related to primitive carbonaceous chondrites that amount to only approximately 2% of meteorite falls. While thousands of micrometeorites have been studied in detail, no micrometeorite has been found so far with an unambiguous achondritic composition and texture. One melted cosmic spherule has a low Fe/Mn ratio similar to that of eucrites, the most common basaltic meteorite group. Here we report on the texture, mineralogy, Rare Earth Elements (REEs) abundance and oxygen isotopic composition of the unmelted Antarctic micrometeorite 99-21-40 that has an unambiguous basaltic origin.

Gounelle, M.↗
NASA NTRS1979

Cosmic ray isotope abundances from chromium to nickel

IRIS, a telescope consisting of a large-area precision Cerenkov detector, scintillators, spark chambers, and a passive stack of Lexan polycarbonate track detectors, was exposed to the primary cosmic radiation for 6.6 sq m sr hr in a balloon flight in 1976. This measurement has yielded the isotopic composition of the iron-group elements Cr, Mn, Fe, and Ni with an average mass resolution of 0.65 amu for the energies 320-500 MeV per amu at the detector. This experiment places the most severe constraints to date on deviation from solar-system composition of the source of the cosmic radiation. Upper limits of 10 percent are placed on the ratios Fe-54/Fe-56 and Fe-58/Fe-56, which are inconsistent with large departures from solar system source composition reported by other workers. The isotopic measurements of Fe and Ni preclude the possibility that these cosmic rays were produced in a single e-process zone. The mean mass of Mn is less than 55, indicating the presence of electron-capture species produced by spallation.

Tarle, G.↗
NASA NTRS1988

Seawater strontium isotopes, acid rain, and the Cretaceous-Tertiary boundary

A large bolide impact at the end of the Cretaceous would have produced significant amounts of nitrogen oxides by shock heating of the atmosphere. The resulting acid precipitation would have increased continental weathering greatly and could be an explanation for the observed high ratio of strontium-87 to strontium-86 in seawater at about this time, due to the dissolution of large amounts of strontium from the continental crust. Spikes to high values in the seawater strontium isotope record at other times may reflect similar episodes.

Macdougall, J. D.↗
NASA NTRS1986

Geochronology and petrogenesis of Apollo 14 very high potassium mare basalts

Rb-Sr, K-Ar, and Sm-Nd isotopic studies were undertaken for two Apollo 14 very high potassium (VHK) highly radiogenic mare basaltic clasts from breccias 14305 and 14168. Rb-Sr data indicate ages of 3.83 + or - 0.08 b.y., and 3.82 + or - 0.12 b.y. for samples 14305 and 14168 respectively, for lambda(Rb-87) = 0.0 139/b.y. Their corresponding initial Sr-87/Sr-86 ratios are nearly identical, as well as their Ar-39 to Ar-40 age spectra, and it is proposed that they were derived from the same flow. The Sm-Nd isotopic data of whole rock and mineral separates for the two VHK basalts define an internal isochrone age of 3.94 + or - 0.16 b.y. for lambda (Sm-147) = 0.00654/b.y. and an initial Nd-143/Nd-144 of 0.50673 + or - 21. The similarity in isotopic ages suggests that VHK basalts crystallized from a melt about 3.85 b.y. ago. VHK basalts show very large Rb/Sr fractionation but no significant Sm/Nd fractionation at the time of crystallization. The source material had a Rb/Sr ratio similar to those of Apollo 14 high-Al mare basalts and a nearly chrondritic Sm/Nd ratio. Basalt/granite interaction was found to be responsible for the extreme enrichments of Rb/Sr and K/La during the formation of VHK basalts. It is concluded that K, Rb-rich components of granitic wall rocks in the highland crust were selectively introduced into ascending hot high-Al mare basaltic magma upon contact.

Shih, C.-Y.↗
DOE OSTI2026

Separation of Hydrogen Using Pd/Ag Membranes: Experimental and Modeling Results with Potential Application to Direct Internal Recycle

Implementation of fusion energy requires processing the deuterium-tritium (D-T) mixture used to fuel the reaction, and separation of hydrogen isotopes from other gases is imperative. Specifically, the separation of hydrogen isotopes from helium is a matter of importance to the fusion fuel cycle community. Initial testing with a palladium-silver (Pd-Ag) membrane indicates that even moderate vacuum (~100 torr permeate pressure) can provide a high degree of separation (>90%) at a high ratio of H 2 to He. Given the presence of He in many fusion systems, a high technology readiness level (TRL) for Q 2 /He (where Q represents any isotope of hydrogen) separations is needed. This study demonstrates the efficacy of H 2 removal from He via permeation and potential applications for direct internal recycle. Modeling will accompany the experimental campaign to generate a predictive capability and quantify the separation performance. Modeling from previous hydrogen permeation studies has demonstrated that the typical Sieverts’ law fails to predict the measured permeation rates at high hydrogen fluxes. Existing models are being refined to integrate the effects of surface phenomena into permeation predictions, which have been expanded to account for mixtures with large ranges of Q 2 concentrations. These data will improve the TRL of permeators as a separation technology for the fusion fuel cycle.

08 HYDROGEN↗
NASA NTRS1993

The Sm-(146,147)-Nd-(142,143) formation interval for the lunar mantle and implications for lunar evolution

Small anomalies in the isotopic abundance of Nd-142 have been measured for two A17 high-Ti basalts, ilmenite basalt 12056, olivine-pigeonite basalt 12039, feldspathic basalt 12038, and two KREEP basalts. These anomalies correlate with Sm-147/Nd-144 for the basalt source regions as calculated from initial Nd-143/Nd-144 ratios in the basalts, and are interpreted to be from decay of Sm-146 (t sub 1/2 = 103 Ma) in distinct lunar mantle reservoirs. A three-stage model for evolution of Nd-143/Nd-144 and Nd-142/Nd-144 yields reservoir Sm-147/Nd-144 ratios which, with the Nd-142/Nd-144 ratios in the basalts, form a 'mantle isochron' giving a lunar mantle formation interval of 94+2230 Ma (2c(rho)). Calculated reservoir Sm/Nd ratios are in the range expected from some earlier models of basalt petrogenesis. The isochron value of Nd-142/Nd-144 at Sm-147/Nd-144 sub CHUR = 0.1967 is within error limits of the average Nd-142/Nd-144 measured for an L6 chondrite, an H5 chondrite, and the Orgueil carbonaceous chondrite. Evolution of Nd-143 and Nd-142 for high-Ti basalt 70135 was modeled precisely, starting from chondritic relative REE and Nd-isotopic abundances and using the initial (Sm-146/Sm-144) sub 0 ratio inferred from a previous study of angrite LEW86010 as the initial solar system value of this parameter. We infer that the initial Sm/Nd ratio in precursor lunar materials was very nearly chondritic (within approximately 8 percent) prior to lunar differentiation.

Nyquist, L. E.↗
DOE OSTI2024

The role of isotope mass on neutral fueling and density pedestal structure in the DIII-D tokamak

Abstract Experimental measurements on DIII-D of hydrogen neutral penetration lengths ( λ n 0 ) on the high field side (HFS) are longer by a factor of 2 than for deuterium consistent with the thermal velocity ratio for neutrals at the same temperature ( v t h H / v t h D = 2 ) . This ratio is constant for both low and high pedestal electron density. At low pedestal density ( n e ∼ 4 × 10 19 m − 3 ) , the neutral penetration length is greater than the density pedestal width for both isotopes, and the additional 40% increase of neutral penetration in hydrogen widens the pedestal by the same amount. As the density pedestal height increases ( n e ∼ 6 × 10 19 m − 3 ) , the neutral penetration lengths drop below the density pedestal widths for both isotopes, and the increased penetration of hydrogen has no increased effect on the pedestal width compared to deuterium. Extrapolating to future reactor-relevant high electron density pedestals, the isotope-mass change in neutral fueling on the HFS from the deepest neutral penetration of hydrogen, to the shortest neutral penetration of tritium will be negligible (0.2–0.4 cm) in comparison to estimates of the density pedestal width (6–8.5 cm).

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
NASA NTRS1994

Solar wind noble gases and nitrogen in metal from lunar soil 68501

Noble gases and N were analyzed in handpicked metal separates from lunar soil 68501 by a combination of step-wise combustions and pyrolyses. Helium and Ne were found to be unfractionated with respect to one another when normalized to solar abundances, for both the bulk sample and for all but the highest temperature steps. However, they are depleted relative to Ar, Kr and Xe by at least a factor of 5. The heavier gases exhibit mass-dependent fractionation relative to solar system abundance ratios but appear unfractionated, both in the bulk metal and in early temperature steps, when compared to relative abundances derived from lunar ilmenite 71501 by chemical etching, recently put forward as representing the abundance ratios in solar wind. Estimates of the contribution of solar energetic particles (SEP) to the originally implanted solar gases, derived from a basic interpretation of He and Ne isotopes, yield values of about 10%. Analysis of the Ar isotopes requires a minimum of 20% SEP, and Kr isotopes, using our preferred composition for solar wind Kr, yield a result that overlaps both these values. It is possible to reconcile the data from these gases if significant loss of solar wind Ar, Kr and presumably Xe has occurred relative to the SEP component, most likely by erosive processes that are mass independent, although mass-dependent losses (Ar greater than Kr greater than Xe) cannot be excluded. If such losses did occur, the SEP contribution to the solar implanted gases must have been no more than a few percent. Nitrogen is a mixture of indigenous meteoritic N, whose isotopic composition is inferred to be relatively light, and implanted solar N, which has probably undergone diffusive redistribution and fractionation. If the heavy noble gases have not undergone diffusive loss, then N/Ar in the solar wind can be inferred to be at least several times the accepted solar ratio. The solar wind N appears, even after correction for fractionation effects, to have a minimum delta N-15 value equal to or greater than +150% and a more probable value equal to or greater than +200%.

Becker, Richard H.↗