Tungsten isotopes and the early evolution of the Moon
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Effective resonance integral measurements of separated tungsten isotopes and natural tungsten relative to gold
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We report the first tungsten isotopic measurements in stardust silicon carbide (SiC) grains recovered from the Murchison carbonaceous chondrite. The isotopes {sup 182,183,184,186}W and {sup 179,180}Hf were measured on both an aggregate (KJB fraction) and single stardust SiC grains (LS+LU fraction) believed to have condensed in the outflows of low-mass carbon-rich asymptotic giant branch (AGB) stars with close-to-solar metallicity. The SiC aggregate shows small deviations from terrestrial (= solar) composition in the {sup 182}W/{sup 184}W and {sup 183}W/{sup 184}W ratios, with deficits in {sup 182}W and {sup 183}W with respect to {sup 184}W. The {sup 186}W/{sup 184}W ratio, however, shows no apparent deviation from the solar value. Tungsten isotopic measurements in single mainstream stardust SiC grains revealed lower than solar {sup 182}W/{sup 184}W, {sup 183}W/{sup 184}W, and {sup 186}W/{sup 184}W ratios. We have compared the SiC data with theoretical predictions of the evolution of W isotopic ratios in the envelopes of AGB stars. These ratios are affected by the slow neutron-capture process and match the SiC data regarding their {sup 182}W/{sup 184}W, {sup 183}W/{sup 184}W, and {sup 179}Hf/{sup 180}Hf isotopic compositions, although a small adjustment in the s-process production of {sup 183}W is needed in order to have a better agreement between the SiC data and model predictions. The models cannot explain the {sup 186}W/{sup 184}W ratios observed in the SiC grains, even when the current {sup 185}W neutron-capture cross section is increased by a factor of two. Further study is required to better assess how model uncertainties (e.g., the formation of the {sup 13}C neutron source, the mass-loss law, the modeling of the third dredge-up, and the efficiency of the {sup 22}Ne neutron source) may affect current s-process predictions.
Effective resonance integrals for separated tungsten isotopes and natural W and Au determined from epicadmium reactivity measurements
We have developed and program-realized a mathematical model of nonstationary separation processes proceeding in cascades of gas centrifuges for separation of multicomponent isotope mixtures. With the help of this model we have calculated the parameters of nonstationary separation processes proceeding in the cascades of gas centrifuges for tungsten isotope separation. It has been shown that the model adequately describes the nonstationary processes in the cascade and is suitable for calculating their parameters during separation of multicomponent isotope mixtures.
Experiments carried out on DIII-D using a novel setup of isotopic tungsten (W) sources in the outer divertor have characterized how the W leakage from this region depends on both the exact source location and edge-localized mode (ELM) behavior. The sources are toroidally-symmetric and poloidally-localized to two regions: (1) the outer strike point (OSP) with natural abundance of W isotopes; and (2) the far-target with highly-enriched 182 W isotopes. With the use of a dual-faced collector probe (CP) in the main scrape-off layer (SOL) near the outside midplane and source-rate spectroscopy, a proxy for divertor impurity leakage is developed herein. Using this proxy, it is found that for the OSP W location, there is a nearly linear increase of leakage with the power across the separatrix ( ), which is consistent with the effect of an increased upstream ion temperature parallel gradient force in the near-SOL; trends in the pedestal density and collisionality are also seen. Conversely, it is found that for the far-target W location leakage falls off rapidly as increases and ELM size decreases, which is suggestive that ELM size plays a role in the leakage from this location. Indications for main SOL W contamination is evidenced by the measurement of large deposition asymmetries on the two opposite CP faces. These measurements are coupled with interpretive modeling showing SOL W accumulation near the separatrix furthest from both targets driven by forces parallel to the magnetic field. This experimental setup, together with the target and upstream W measurements, provides information on the transport from different divertor W source locations and leakage. These studies help to elucidate the physics driving divertor impurity source rates and leakage, with and without ELMs, and provide better insight on the link in the chain connecting wall impurity sources to core impurity levels in magnetic fusion devices.
Progressive dissolution of the Murchison carbonaceous chondrite with acids of increasing strengths reveals large internal W isotope variations that reflect a heterogeneous distribution of s- and r-process W isotopes among the components of primitive chondrites. At least two distinct carriers of nucleosynthetic W isotope anomalies must be present, which were produced in different nucleosynthetic environments. The co-variation of {sup 182}W/{sup 184}W and {sup 183}W/{sup 184}W in the leachates follows a linear trend that is consistent with a mixing line between terrestrial W and a presumed s-process-enriched component. The composition of the s-enriched component agrees reasonably well with that predicted by the stellar model of s-process nucleosynthesis. The co-variation of {sup 182}W/{sup 184}W and {sup 183}W/{sup 184}W in the leachates provides a means for correcting the measured {sup 182}W/{sup 184}W and {sup 182}W/{sup 183}W of Ca-Al-rich inclusions (CAI) for nucleosynthetic anomalies using the isotopic variations in {sup 183}W/{sup 184}W. This new correction procedure is different from that used previously, and results in a downward shift of the initial {epsilon}{sup 182}W of CAI to -3.51 {+-} 0.10 (where {epsilon}{sup 182}W is the variation in 0.01% of the {sup 182}W/{sup 183}W ratio relative to Earth's mantle). This revision leads to Hf-W model ages of core formation in iron meteorite parent bodies that are {approx}2 Myr younger than previously calculated. The revised Hf-W model ages are consistent with CAI being the oldest solids formed in the solar system, and indicate that core formation in some planetesimals occurred within {approx}2 Myr of the beginning of the solar system.
The addition of isotopically enriched taggants to material at the front end of the nuclear fuel cycle could be a powerful tool used to assist law enforcement authorities should material outside of regulatory control be found. Two potential candidates for this purpose are molybdenum (Mo) and tungsten (W) as both elements have five or more stable isotopes and are trace elements contained within nuclear fuel. So there is a concern that Mo and W could undergo isotope fractionation during processes like uranium enrichment and to date, it is unknown if nuclear fuels have natural Mo and W isotope compositions. If Mo and W isotopic variability is present in nuclear fuels, this would hinder the use of these elements as isotopic taggants because it would be difficult to discern the original taggant isotope composition with high confidence. Therefore, a set of 16 low enriched uranium (LEU) fuel pellets from US commercial producers was analyzed using multi collector-inductively coupled plasma mass spectrometry (MC-ICPMS) to determine Mo and W isotope compositions (i.e., 94 Mo/ 92 Mo, 95 Mo/ 92 Mo, 96 Mo/ 92 Mo, 97 Mo/ 92 Mo, 98 Mo/ 92 Mo, 183 W/ 182 W, 184 W/ 182 W, and 186 W/ 182 W). Relative to terrestrial standards, LEU fuel pellets have variable Mo and W isotope compositions, thereby complicating the use of these elements as isotopically enriched taggants. As such, this work demonstrates that the isotope composition of any potential taggant must be well characterized in the base nuclear fuel prior to any taggant addition. Furthermore, these results suggest that Mo and W are not ideal candidates for isotopically enriched taggants.
A new set of measurements for the total and capture cross section determination of W isotopes was done using GELINA (GEel LINear Accelerator), a neutron Time-Of-Flight facility at the Institute for Reference Materials and Measurements (IRMM). Measuring stations at different flight path lengths were used in order to cover a broad neutron energy range with high resolution demands. Experimental techniques adopted for both transmission and capture measurements are well established using a (6)Li glass detector and C(6)D(6) scintillation arrays as detections systems respectively., As target samples highly enriched (182,183,184,186)W metallic discs were used.
Neutron capture cross section measurements on tungsten 183, 184, and 186 using totally absorbing gamma ray detector
Here we report the Moon most likely formed as the result of a collision between the proto-Earth and a differentiated body possibly the size of Mars (Cameron and Benz, 1991; Hartmann and Davis, 1975). The enormous amount of energy released by this giant impact caused widespread melting on the proto-Earth and the ejection of material into Earth’s orbit from which the Moon subsequently accreted. Upon accretion of the Moon, the lunar mantle underwent global silicate differentiation most likely facilitated by a lunar magma ocean (e.g. Wood et al., 1970). Magma ocean crystallization likely produced the wide diversity of lunar source rocks and involved the successive crystallization of mafic cumulates consisting of olivine and pyroxene, followed by crystallization of plagioclase which floated to the lunar surface to form the lunar crust consisting of ferroan anorthosites (FAN). Lastly, the residual liquid of the lunar magma ocean represents a separate component within the Moon termed KREEP (enriched in Potassium K, Rare Earth Elements, and Phosphorous). Re-melting of these magma ocean crystallization products of the low-Ti and high-Ti mare basalt source regions as well as the formation of Mg-suite lunar highland rocks.
Here, the giant impact model of lunar origin predicts that the Moon mainly consists of impactor material. As a result, the Moon is expected to be isotopically distinct from the Earth, but it is not. To account for this unexpected isotopic similarity of the Earth and Moon, several solutions have been proposed, including (i) post-giant impact Earth–Moon equilibration, (ii) alternative models that make the Moon predominantly out of proto-Earth mantle, and (iii) formation of the Earth and Moon from an isotopically homogeneous disk reservoir. Here we use W isotope systematics of lunar samples to distinguish between these scenarios. We report high-precision 182 W data for several low-Ti and high-Ti mare basalts, as well as for Mg-suite sample 77215, and lunar meteorite Kalahari 009, which complement data previously obtained for KREEP-rich samples. In addition, we utilize high-precision Hf isotope and Ta/W ratio measurements to empirically quantify the superimposed effects of secondary neutron capture on measured 182 W compositions. Our results demonstrate that there are no resolvable radiogenic 182 W variations within the Moon, implying that the Moon differentiated later than 70 Ma after Solar System formation. In addition, we find that samples derived from different lunar sources have indistinguishable 182 W excesses, confirming that the Moon is characterized by a small, uniform ~+26 parts-per-million excess in 182 W over the present-day bulk silicate Earth. This 182W excess is most likely caused by disproportional late accretion to the Earth and Moon, and after considering this effect, the pre-late veneer bulk silicate Earth and the Moon have indistinguishable 182 W compositions. Mixing calculations demonstrate that this Earth–Moon 182 W similarity is an unlikely outcome of the giant impact, which regardless of the amount of impactor material incorporated into the Moon should have generated a significant 182 W excess in the Moon. Consequently, our results imply that post-giant impact processes might have modified 182 W, leading to the similar 182 W compositions of the pre-late veneer Earth's mantle and the Moon.
Chondrules and matrix from carbonaceous chondrites exhibit complementary nucleosynthetic W isotope anomalies that result from the depletion of a metallic s-process carrier in the chondrules, and the enrichment of this carrier in the matrix. The complementarity is difficult to reconcile with an origin of chondrules in protoplanetary impacts and also with models in which chondrules and matrix formed independently of each other in distinct regions of the disk. Instead, the complementarity indicates that chondrules formed by localized melting of dust aggregates in the solar nebula. The Hf–W ages for metal-silicate fractionation in CV and CR chondrites are 2.2 ± 0.8 Ma and 3.6 ± 0.6 Ma after formation of Ca-Al-rich inclusions, and are indistinguishable from Al–Mg ages for CV and CR chondrules. The good agreement between these ages strongly suggests that 26 Al was homogeneously distributed in the solar protoplanetary disk and that therefore Al–Mg ages are chronologically meaningful. The concordant Al–Mg and Hf–W ages reveal that chondrule formation (as dated by Al–Mg) was associated with metal-silicate fractionation (as dated by Hf–W), both within a given chondrite but also among the different subgroups of ordinary chondrites. These age data indicate that chondrules from a given chondrite group formed in a narrow time interval of <1 Ma, and that chondrule formation and chondrite accretion were closely linked in time and space. The rapid accretion of chondrules into a chondrite parent body is consistent with the isotopic complementarity, which requires that neither chondrules nor matrix were lost prior to chondrite accretion. Here combined, these observations suggest that chondrule formation was an important step in the accretion of planetesimals.
High-precision W isotopic analyses by Harper and Jacobsen indicate the W-182/W-183 ratio in the Toluca iron meteorite is shifted by -(3.0 +/- 0.9) x 10(exp -4) relative to a terrestrial standard. Possible causes of this shift are neutron-capture reactions on W during Toluca's approximately 600-Ma exposure to cosmic ray particles or radiogenic growth of W-182 from 9-Ma Hf-182 in the silicate portion of the Earth after removal of W to the Earth's core. Calculations for the rates of neutron-capture reactions on W isotopes were done to study the first possibility. The LAHET Code System (LCS) which consists of the Los Alamos High Energy Transport (LAHET) code and the Monte Carlo N-Particle(MCNP) transport code was used to numerically simulate the irradiation of the Toluca iron meteorite by galactic-cosmic-ray (GCR) particles and to calculate the rates of W(n, gamma) reactions. Toluca was modeled as a 3.9-m-radius sphere with the composition of a typical IA iron meteorite. The incident GCR protons and their interactions were modeled with LAHET, which also handled the interactions of neutrons with energies above 20 MeV. The rates for the capture of neutrons by W-182, W-183, and W-186 were calculated using the detailed library of (n, gamma) cross sections in MCNP. For this study of the possible effect of W(n, gamma) reactions on W isotope systematics, we consider the peak rates. The calculated maximum change in the normalized W-182/W-183 ratio due to neutron-capture reactions cannot account for more than 25% of the mass 182 deficit observed in Toluca W.
Abstract not provided.
With the aid of experimental data on the level densities in the even-odd tungsten isotopes {sup 183,185,187}W as determined in the respective (n, 2{rho}) reactions, the ratio of the cross section for the interaction of an excited nucleus with a neutron to its counterpart calculated on the basis of the optical model of the nucleus was obtained from the spectra of evaporated neutrons in the reaction {sup 181}Ta(p, n){sup 181}W. A significant local increase in this ratio is qualitatively interpreted as that which is due to the possible increase in the penetrability of the nuclear surface for nucleon reaction products because of the effect of phonon-type excitations. Sources of possible nonstandard systematic errors in experimentally determining the level density in an arbitrary nucleus at energies below the nucleon binding energy B{sub n} are analyzed. The extraction of information from the distribution of the intensities of cascades belonging to the nucleon and photon type is simulated. The resulting information may be highly reliable if use is made of the entire body of experimental data on the nucleus under analysis.
Oak Ridge National Laboratory (ORNL) has recently completed the resonance parameter evaluation of four tungsten isotopes, i.e., 182,183,184,186 W, in the neutron energy range of thermal up to several keV. This nuclear data work was performed with support from the US Nuclear Criticality Safety Program (NCSP) in an effort to provide improved tungsten cross section and covariance data for criticality safety analyses. The evaluation methodology uses the Reich-Moore approximation of the R-matrix formalism of the code SAMMY to fit high-resolution measurements performed in 2010 and 2012 at the Geel linear accelerator facility (GELINA), as well as other experimental data sets on natural tungsten available in the EXFOR library. In the analyzed energy range, this work nearly doubles the resolved resonance region (RRR) present in the latest US nuclear data library ENDF/B-VII.1. In view of the interest in tungsten for distinct types of nuclear applications and the relatively homogeneous distribution of the isotopic tungsten—namely, 182 W(26.5%), 183 W(14.31%), 184 W(30.64%), and 186 W(28.43%) - the completion of these four evaluations represents a significant contribution to the improvement of the ENDF library. This paper presents an overview of the evaluated resonance parameters and related covariances for total and capture cross sections on the four tungsten isotopes.