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At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Simultaneous Iron and Nickel Isotopic Analyses of Presolar Silicon Carbide Grains.

Aside from recording stellar nucleosynthesis, a few elements in presolar grains can also provide insights into the galactic chemical evolution (GCE) of nuclides. We have studied the carbon, silicon, iron, and nickel isotopic compositions of presolar silicon carbide (SiC) grains from asymptotic giant branch (AGB) stars to better understand GCE. Since only the neutron-rich nuclides in these grains have been heavily influenced by the parent star, the neutron-poor nuclides serve as GCE proxies. Using CHILI, a new resonance ionizationmass spectrometry (RIMS) instrument, we measured 74 presolar SiC grains for all iron and nickel isotopes. With the CHARISMA instrument, 13 presolar SiC grains were analyzed for iron isotopes. All grains were also measured by NanoSIMS for their carbon and silicon isotopic compositions. A comparison of the measured neutron-rich isotopes with models for AGB star nucleosynthesis shows that our measurements are consistent with AGB star predictions for low-mass stars between half-solar and solar metallicity. Furthermore, our measurements give an indication on the Ne-22(alpha, n)Mg-25 reaction rate. In terms of GCE, we find that the GCE-dominated iron and nickel isotope ratios, Fe-54/Fe-56 and Ni-60/Ni-58, correlate with their GCE-dominated counterpart in silicon, Si-29/Si-28. The measured GCE trends include the Solar System composition, showing that the Solar System is not a special case. However, as seen in silicon and titanium, many presolar SiC grains are more evolved for iron and nickel than the Solar System. This confirms prior findings and agrees with observations of large stellar samples that a simple age-metallicity relationship for GCE cannot explain the composition of the solar neighborhood. (C) 2017 Elsevier Ltd. All rights reserved.

galactic chemical evolution↗
DOE OSTI2017

Iron and nickel isotope compositions of presolar silicon carbide grains from supernovae

Here we report the carbon, silicon, iron, and nickel isotope compositions of twenty-five presolar SiC grains of mostly supernova (SN) origin. The iron and nickel isotope compositions were measured with the new Chicago Instrument for Laser Ionization, CHILI, which allows the analysis of all iron and nickel isotopes without the isobaric interferences that plagued previous measurements with the NanoSIMS. Despite terrestrial iron and nickel contamination, significant isotopic anomalies in 54 Fe/ 56 Fe, 57 Fe/ 56 Fe, 60 Ni/ 58 Ni, 61 Ni/ 58 Ni, 62 Ni/ 58 Ni, and 64 Ni/ 58 Ni were detected in nine SN grains (of type X). Combined multi-isotope data of three grains with the largest nickel isotope anomalies (>100% or <-100% in at least one isotope ratio, when expressed as deviation from the solar value) are compared with the predictions of two SN models, one with and one without hydrogen ingestion in the He shell prior to SN explosion. One grain's carbon-silicon-iron-nickel isotope composition is consistent with the prediction of the model without hydrogen ingestion, whereas the other two grains' isotope anomalies could not be reproduced using either SN models. The discrepancies between the measured isotope compositions and model predictions may indicate element fractionation in the SN ejecta prior to or during grain condensation, and reiterate the need for three-dimensional SN models.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS1993

Iron and nickel isotopic mass fractionation in deep-sea spherules

Magnetite-wuestite spherules collected from deep-sea sediments are thought to have originally been Fe-Ni metal particles at the top of the atmosphere that were oxidized and melted during entry into the earth's atmosphere. Some likely sources for the metal particles are Fe-Ni interplanetary dust particles (IDP's) and metal or sulfide from stony IDP's that separated after melting. Davis et al. reported that four of these spherules are enriched in the heavy isotopes of iron, with enrichments of 8-23%/amu. We have developed a technique for analysis of both iron and nickel isotopes on the same ion microprobe spot and have applied this technique to a number of deep-sea spherules in order to better understand the processes leading to isotopic mass fractionation. Eight spherules show iron and nickel isotopic mass fractionation, with iron and nickel enriched in the heavy isotopes by 10-19%/amu and 4-32%/amu, respectively. If the mass fractionations are due to Rayleigh fractionation during evaporation, these spherules lost 76-94% of their original mass. We have analyzed the four magnetite-wuestite spherules for which iron isotopic data were reported by Davis et al. as well as four new spherules.

Davis, Andrew M.↗
DOE OSTI2018

Impact of Tensor Interaction on Beta-Delayed Neutron Emission from Neutron-Rich Nickel Isotopes

The Skyrme energy density functional including tensor interaction is used to describe microscopically multineutron delayed-neutron emission accompanying beta decay of even–even neutron-rich nickel isotopes of mass number in the range of A = 74−80. The respective calculations are performed in the quasiparticle random-phase approximation with allowance for the two-phonon components of the wave function for states of the daughter nucleus. The properties of the lowest quadrupole excitation of {sup 74,76,78,80}Ni are also studied. It is shown that a decrease in the strength of neutron–proton tensor interaction leads to a substantial hindrance of beta decay and to an increase in the probability for delayedneutron emission.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2017

Large mass-dependent nickel isotope fractionation in Orgueil carbonate: implications for 60 Fe in the early Solar System

Iron-60 is a uniquely important short-lived radionuclide, because it cannot be produced by particle irradiation, and thus, high initial 60 Fe abundances inferred in early-formed Solar System objects must be attributed to injection from a stellar source. Estimates of the initial 60 Fe/ 56 Fe ratio range over a factor of 60 from 1×10 –8 , as determined by high-precision analyses of bulk meteorites, to ~6×10 –7 , from in-situ measurements of high Fe/Ni phases. The reasons for this discrepancy are not clear. To investigate this, we used the UCLA ims1270 and ims1290 ion microprobes to analyze Orgueil carbonate grains that exhibit very high Fe/Ni ratios and are known from 53 Mn- 53 Cr systematics to have formed within ~5 My of CAIs. Our SIMS investigations found two Orgueil breunnerite grains that show apparent 60 Ni excesses. Correlations with Fe/Ni are generally not well defined, but the data imply a relatively high 60 Fe/ 56 Fe ratio of ~10 –7 at the time of carbonate formation. To test the accuracy of the SIMS nickel isotope measurements, we analyzed the same carbonate grains with RIMS using CHILI, the CHicago Instrument for Laser Ionization. The data obtained on the Orgueil carbonates reveal correlations between 62 Ni/ 58 Ni and 60 Ni/ 58 Ni that are strictly mass-dependent. The range in mass fractionation is very large, up to ~35‰/u, predominantly favoring the light isotopes. Our RIMS measurements conclusively demonstrate the occurrence of mass-fractionated nickel in meteorite samples. This isotopic fractionation is large enough that elevated 60 Ni/ 62 Ni ratios could be incorrectly attributed to 60 Fe decay if this mass fractionation is not accurately accounted for.

58 GEOSCIENCES↗
DOE OSTI2026

Optimizing a chemical cleaning protocol to determine the nickel isotopic composition of ancient seawater from carbonates

Reconstructing the ancient marine cycle of Ni, a trace metal in the oceans essential to enzymes regulating the C, N, and O cycles, would inform how Ni bioavailability shaped early life. The Ni isotopic composition of seawater (δ 60 Ni SW ) through time could provide insight, but this approach requires sedimentary archives that faithfully record δ 60 Ni SW . Carbonates are an often-used record of seawater chemistry, but contaminants could bias the measured δ 60 Ni of bulk sediment. To isolate the true carbonate-bound δ 60 Ni signal, we optimized a chemical cleaning protocol designed to minimize non‑carbonate Ni contributions and maximize carbonate recovery. We analyzed ODP Site 1007 sediments and evaluated oxidative and reductive pre-cleaning steps and carbonate dissolution protocols. Our results show that only reductive cleaning significantly altered the subsequent carbonate leachate composition, lowering Ni/Ca ratios by up to 60% and δ 60 Ni values by as much as 0.4 ‰. In contrast, δ 60 Ni values were largely insensitive to premature carbonate dissolution during pre-cleaning or to partial leaching of silicates during carbonate dissolution, even at higher acid molarities or longer reaction times. We recommend an evidence-based protocol that removes hydro-soluble salts and clays, applies reductive cleaning and oxidative cleaning for certain sample compositions, and dissolves carbonate using 0.5 M acetic acid, adjusted to pH 5. Using these results, we infer a ∼ 0.9 ‰ Ni isotopic fractionation between chemically cleaned deep-water carbonates (+0.4 ± 0.1 ‰) and deep seawater. This method development is a key step toward accurately reconstructing ancient marine Ni cycles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Effects of helium on irradiation response of reduced-activation ferritic-martensitic steels: Using nickel isotopes to simulate fusion neutron response

Understanding the effects of helium on microstructures and mechanical properties of reduced-activation ferritic-martensitic steels is important to use of these steels in fusion reactor structures. The 9Cr-2WVTa steels were doped with 58Ni and 60Ni isotopes at 2 weight percent to control the rate of transmutation helium generation. The samples were irradiated in the High Flux Isotope Reactor to ~24 displacements per atom at nominal temperatures of 300, 400, and 500°C, producing 228 and 7 atomic parts-per-million helium in the 58 Ni- and 60 Ni-doped samples, respectively. Transmission electron microscopy revealed a variety of precipitates and the radiation-induced dislocation loops and cavities (voids or helium bubbles). Tensile tests of the irradiated samples at the irradiation temperatures showed radiation-induced hardening at 300°C and radiation-induced softening at 400°C. Analysis indicates that the hardening primarily originated from the loops and cavities. The 58 Ni-doped samples had greater strengthening contributions from loops and cavities, leading to higher hardening with lower ductility than the 60 Ni-doped samples. The greater helium production of 58 Ni did not show pronounced reductions in ductility of the samples.

36 MATERIALS SCIENCE↗
DOE OSTI2016

CHILI – the Chicago Instrument for Laser Ionization – a new tool for isotope measurements in cosmochemistry

We describe CHILI, the Chicago Instrument for Laser Ionization, a new resonance ionization mass spectrometer developed for isotopic analysis at high spatial resolution and high sensitivity of small samples like contemporary interstellar dust grains returned by the Stardust spacecraft. We explain how CHILI addresses the technical challenges associated with such analyses by pushing most technical specifications towards their physical limits. As an initial demonstration, after many years of designing and developing CHILI, we have analyzed presolar silicon carbide grains for their isotopic compositions of strontium, zirconium, and barium. Subsequently, after further technical improvements, we have used CHILI to analyze, for the first time without interference, all stable isotopes of iron and nickel simultaneously in presolar silicon carbide grains. With a special timing scheme for the ionization lasers, we separated iron and nickel isotopes in the time-of-flight spectrum such that the isobaric interference between Fe-58 and Ni-58 was resolved. In-depth discussion of the astrophysical implications of the presolar grain results is deferred to dedicated later publications. Here we focus on the technical aspects of CHILI, its status quo, and further developments necessary to achieve CHILI's ultimate goals, similar to 10 nm lateral resolution and 30-40% useful yield.

Stephan, Thomas (ORCID:0000000163778731)↗
DOE OSTI2024

Synthesis and characterization of isotopically barcoded nickel, molybdenum, and tungsten taggants for intentional nuclear forensics

Intentional nuclear forensics is a concept wherein the deliberate addition of benign and persistent material signatures to nuclear material can be used to reduce the time between the discovery of material outside of regulatory control and determination of its original provenance. One concept within intentional nuclear forensics involves the use of perturbed stable isotopes to generate unique isotope ratio “barcodes” to encode information (e.g., production batch, location, etc.) and track material throughout the nuclear fuel cycle. Synthesis of taggant species of nickel (Ni), molybdenum (Mo), and tungsten (W) was undertaken via a double-spike mechanism, wherein two highly enriched isotopes of interest per elemental taggant were mixed to form an enriched “double-spike” which was subsequently isotopically diluted with bulk material having a natural isotopic composition. Two taggant species perturbing isotopic ratios, alpha (α) and beta (β), for each of Ni, Mo, and W were synthesized. Independent measurements of double spikes and alpha and beta taggant species agreed within uncertainty and are clearly resolvable from natural compositions. High-precision analyses were independently performed by MC-ICP-MS at two U.S. National Laboratories, with consensus values and uncertainties calculated for all samples. Observed isotopic perturbations in the final taggant species measured on the order of hundreds to thousands of permille (‰) with respect to natural for isotope ratios of interest (e.g., 60 Ni/ 58 Ni, 100 Mo/ 98 Mo, 186 W/ 183 W). Discrepancies between modeled and measured isotopic compositions were observed and are largely attributed to imprecise vendor assay values for starting materials. Using measured starting material compositions as inputs for the mixing model improved the level of agreement between predicted and measured α and β taggant isotope ratios. Overall, characterization of all taggant species demonstrates that this “barcode” concept could have viability for use in nuclear forensics. Finally, it is expected that for any two-isotope mixing array dozens of isotopic barcodes could be encoded into a material system and subsequently resolved utilizing modern mass spectrometric methods.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗
DOE OSTI2018

New Constraints on the Abundance of 60 Fe in the Early Solar System

Establishing the abundance of the extinct radionuclide 60 Fe (half-life 2.62 Ma) in the early solar system is important for understanding the astrophysical context of solar system formation. While bulk measurements of early solar system phases show a low abundance consistent with galactic background, some in situ measurements by secondary ion mass spectrometry (SIMS) imply a higher abundance, which would require injection from a nearby supernova (SN). In this paper, we present in situ nickel isotopic analyses by resonance ionization mass spectrometry (RIMS) in a chondrule from the primitive meteorite Semarkona (LL3.00). The same chondrule had been previously analyzed by SIMS. Despite improved precision compared to SIMS, the RIMS nickel isotopic data do not reveal any resolved excesses of 60 Ni that could be unambiguously ascribed to in situ 60 Fe decay. Linear regression of 60 Ni/ 58 Ni versus 56 Fe/ 58 Ni yields an initial 60 Fe/ 56 Fe ratio for this chondrule of (3.8 ± 6.9) × 10 -8 , which is consistent with both the low initial value found by bulk measurements and the low end of the range of initial ratios inferred from some in situ work. The same regression also gives a solar initial 60 Ni/ 58 Ni ratio, which shows that this sample was not disturbed by nickel mobilization, thus agreeing with a low initial 60 Fe/ 56 Fe ratio. These findings agree with a re-evaluation of previous SIMS measurements of the same sample. Finally, supernova injection of 60 Fe into the solar system or its parental cloud material is therefore not necessary to account for the measured solar system's initial amount of 60 Fe.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2024

Microscopic optical potentials for medium-mass isotopes derived at the first order of Watson multiple-scattering theory

We perform a first-principles calculation of optical potentials for nucleon elastic scattering off medium-mass isotopes. Fully based on a saturating chiral Hamiltonian, the optical potentials are derived by folding nuclear density distributions computed with self-consistent Green's function theory with a nucleon-nucleon t matrix computed with a consistent chiral interaction. The dependence on the folding interaction as well as the convergence of the target densities are investigated. Numerical results are presented and discussed for differential cross sections and analyzing powers, with focus on elastic proton scattering off calcium and nickel isotopes. Our optical potentials generally show a remarkable agreement with the available experimental data for laboratory energies in the range 65–200 MeV. We study the evolution of the scattering observables with increasing proton-neutron asymmetry by computing theoretical predictions of the cross section and analyzing power over the calcium and nickel isotopic chains. Published by the American Physical Society 2024

Physics↗
DOE OSTI2014

The light curve of SN 1987A revisited: constraining production masses of radioactive nuclides

We revisit the evidence for the contribution of the long-lived radioactive nuclides {sup 44}Ti, {sup 55}Fe, {sup 56}Co, {sup 57}Co, and {sup 60}Co to the UVOIR light curve of SN 1987A. We show that the V-band luminosity constitutes a roughly constant fraction of the bolometric luminosity between 900 and 1900 days, and we obtain an approximate bolometric light curve out to 4334 days by scaling the late time V-band data by a constant factor where no bolometric light curve data is available. Considering the five most relevant decay chains starting at {sup 44}Ti, {sup 55}Co, {sup 56}Ni, {sup 57}Ni, and {sup 60}Co, we perform a least squares fit to the constructed composite bolometric light curve. For the nickel isotopes, we obtain best fit values of M({sup 56}Ni) = (7.1 ± 0.3) × 10{sup –2} M {sub ☉} and M({sup 57}Ni) = (4.1 ± 1.8) × 10{sup –3} M {sub ☉}. Our best fit {sup 44}Ti mass is M({sup 44}Ti) = (0.55 ± 0.17) × 10{sup –4} M {sub ☉}, which is in disagreement with the much higher (3.1 ± 0.8) × 10{sup –4} M {sub ☉} recently derived from INTEGRAL observations. The associated uncertainties far exceed the best fit values for {sup 55}Co and {sup 60}Co and, as a result, we only give upper limits on the production masses of M({sup 55}Co) < 7.2 × 10{sup –3} M {sub ☉} and M({sup 60}Co) < 1.7 × 10{sup –4} M {sub ☉}. Furthermore, we find that the leptonic channels in the decay of {sup 57}Co (internal conversion and Auger electrons) are a significant contribution and constitute up to 15.5% of the total luminosity. Consideration of the kinetic energy of these electrons is essential in lowering our best fit nickel isotope production ratio to [{sup 57}Ni/{sup 56}Ni] = 2.5 ± 1.1, which is still somewhat high but is in agreement with gamma-ray observations and model predictions.

79 ASTRONOMY AND ASTROPHYSICS↗