Tungsten Isotopes Research Articles

182W evidence for core-mantle interaction in the source of mantle plumes

Tungsten isotopes are the ideal tracers of core-mantle chemical interaction. Given that W is moderately siderophile, it preferentially partitioned into the Earth’s core during its segregation, leaving the mantle depleted in this element. In contrast, Hf is lithophile, and its short-lived radioactive isotope 182Hf decayed entirely to 182W in the mantle after metal-silicate segregation. Therefore, the 182W isotopic composition of the Earth’s mantle and its core are expected to differ by about 200 ppm. Here, we report new high precision W isotope data for mantle-derived rock samples from the Paleoarchean Pilbara Craton, and the Reunion Island and the Kerguelen Archipelago hotspots. Together with other available data, they reveal a temporal shift in the 182W isotopic composition of the mantle that is best explained by core-mantle chemical interaction. Core-mantle exchange might be facilitated by diffusive isotope exchange at the core-mantle boundary, or the exsolution of W-rich, Si-Mg-Fe oxides from the core into the mantle. Tungsten-182 isotope compositions of mantle-derived magmas are similar from 4.3 to 2.7 Ga and decrease afterwards. This change could be related to the onset of the crystallisation of the inner core or to the initiation of post-Archean deep slab subduction that more efficiently mixed the mantle.

Изменение состава ионного тока в процессе полевого испарения вольфрама при высоких температурах

Steady-state field evaporation of tungsten at high temperatures (T ~ 2000 K) has been studied using a magnetic mass spectrometer equipped with the field ion source. Only low-charged ions (W+2 and W+) have been observed in the course of evaporation. The distribution of the ion currents by tungsten isotopes correspondents to standart isotopic ratio for natural tungsten. Some deviations from standart isotopic ratio were observed owing to fluctuations and unstable nature of evaporation process. O.L. Golubev, N.M. Blashenkov

Tungsten isotopes in mantle plumes: Heads it's positive, tails it's negative

The lowermost mantle is driven to Earth's surface by mantle plumes, providing a volcanic record of its structure and composition. Plumes comprise a head and tail, which melt to form large igneous provinces (LIPs) and ocean island basalts (OIBs), respectively. Recent analyses have shown that LIPs and OIBs exhibit tungsten (W) isotope heterogeneity that was created in the first ∼60 million years of our solar system's evolution. Moreover, the isotopic signature found in LIPs differs to that found in OIBs, revealing that the melt products of plume heads must be dominated by a different ancient mantle reservoir to that of plume tails. However, existing geodynamical studies suggest that plume heads and tails sample the same deep-mantle source region and, therefore, cannot account for any systematic differences in composition. Here, we present a suite of numerical simulations of thermo-chemical plumes and an isotopic model for W sources in the mantle. Our results demonstrate that the W isotope systematics of LIPs and OIBs can, under certain conditions, arise as a dynamical consequence of plumes forming in a heterogeneous, thermo-chemical boundary layer. We find that ultra low-velocity zones (ULVZs), which sit on the core–mantle boundary (CMB), likely contribute to the chemical diversity observed in OIBs but not LIPs, while any dense components residing inside large low shear-wave velocity provinces (LLSVPs) may contribute to both. This study places geochemical observations from Earth's surface in a geodynamically consistent framework and illuminates their relationship with seismically imaged features of the deep mantle.

Excitation Function of (n,α) Reactions of Hafnium and Tungsten Isotopes for Fusion Reactor Technology

Excitation Function of (n,α) Reactions of Hafnium and Tungsten Isotopes for Fusion Reactor Technology

Alpha and cluster decay half-lives in Tungsten isotopes: A microscopic analysis

Alpha and cluster decay half-lives of Tungsten (W) isotopes in the range between 2p drip line and beta stability line are studied. The sensitivity of different Skyrme parametrizations in predicting the alpha decay and probable cluster decay modes from W isotopes have been analysed. The half-lives are calculated using Universal Decay Law (UDL). Predicted half-lives are compared with Effective Liquid Drop Model (ELDM) and also with available experimental values. The use of harmonic oscillator (HO) and transformed harmonic oscillator (THO) basis do not produce much differences in the results. The study also revealed the role of neutron shell closure in cluster decay process.

Mathematical Modeling of Nonstationary Separation Processes in a Cascade of Gas Centrifuges for Separation of Tungsten Isotopes

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.

Motion of W and He atoms during formation of W fuzz

Measurements are conducted to identify the motion of tungsten and helium atoms during the formation of tungsten fuzz. In a first series of experiments the mobility of helium within the growing fuzz was measured by adding 3He to the different stages of plasma exposure under conditions that promoted tungsten fuzz growth. Ion beam analysis was used to quantify the amount of 3He remaining in the samples following the plasma exposure. The results indicate that the retention of helium in bubbles within tungsten is a dynamic process with direct implantation rather than diffusion into the bubbles, best describing the motion of the helium atoms. In the second experiment, an isotopically enriched layer of tungsten (~92.99% 182W) is deposited on the surface of a bulk tungsten sample with the natural abundance of the isotopes. This sample is then exposed to helium plasma at the conditions necessary to support the formation of tungsten ‘fuzz’. Depth profiles of the concentration of each of the tungsten isotopes are obtained using secondary ion mass spectrometry (SIMS) before and after the plasma exposure. The depth profiles clearly show mixing of tungsten atoms from the bulk sample toward the surface of the fuzz. This supports a physical picture of the dynamic behavior of helium bubbles which, also, causes an enhanced mixing of tungsten atoms.

No 182W excess in the Ontong Java Plateau source

Small-scale W isotope variations in ancient and modern terrestrial rocks provide insights into Earth's accretion and early differentiation history as well as the long-term evolution of the Earth's mantle. Tungsten isotope studies on such rocks have exploited advances in mass spectrometry, both NTIMS and MC-ICPMS, which now permit the determination of W isotope ratios at unprecedented precision. While W isotope studies performed in different labs by MC-ICPMS and NTIMS generally exhibit excellent agreement, obtaining accurate W isotope data at this level of precision remains analytically challenging. For example, a recent NTIMS study reported a relatively large, +24 ppm excess in 182W/184W for a Phanerozoic sample from the Ontong Java Plateau (OJP), but no such 182W/184W anomaly was found in another study by MC-ICPMS. The present study aims to resolve the discrepancy between these two previous studies, and more generally to evaluate the agreement between different recent W isotope studies by NTIMS and MC-ICPMS. To this end, we report new W isotope data for OJP drill core samples obtained by MC-ICPMS. The OJP samples analyzed here exhibit no resolvable 182W/184W excess relative to the standards and most terrestrial rocks. Moreover, the OJP samples as well as the terrestrial rock standards analyzed here exhibit small but variable W isotope variations for ratios involving 183W, producing coupled variations in both ‘radiogenic’ (i.e., 182W/183W) and ‘non-radiogenic’ (i.e., 183W/184W) ratios. These W isotope variations are analytical in origin, induced during sample preparation, and very likely caused by a nuclear field shift isotope fractionation affecting primarily the odd isotope (183W). The recently reported 182W excess for an OJP sample may result from this nuclear field shift effect, as the NTIMS analyses had to rely on a double normalization involving the 183W/184W ratio. More generally, these results demonstrate that using 183W data from any MC-ICPMS or NTIMS study requires a careful quantification of any potential analytical 183W effect. Nevertheless, once such effects are taken into account, then both 182W/184W and 183W/184W can accurately be determined to a very high level of precision.

Hadean silicate differentiation preserved by anomalous 142Nd/144Nd ratios in the Réunion hotspot source.

Active volcanic hotspots can tap into domains in Earth's deep interior that were formed more than two billion years ago. High-precision data on variability in tungsten isotopes have shown that some of these domains resulted from differentiation events that occurred within the first fifty million years of Earth history. However, it has not proved easy to resolve analogous variability in neodymium isotope compositions that would track regions of Earth's interior whose composition was established by events occurring within roughly the first five hundred million years of Earth history. Here we report 142Nd/144Nd ratios for Réunion Island igneous rocks, some of which are resolvably either higher or lower than the ratios in modern upper-mantle domains. We also find that Réunion 142Nd/144Nd ratios correlate with helium-isotope ratios (3He/4He), suggesting parallel behaviour of these isotopic systems during very early silicate differentiation, perhaps as early as 4.39 billion years ago. The range of 142Nd/144Nd ratios in Réunion basalts is inconsistent with a single-stage differentiation process, and instead requires mixing of a conjugate melt and residue formed in at least one melting event during the Hadean eon, 4.56 billion to 4 billion years ago. Efficient post-Hadean mixing nearly erased the ancient, anomalous 142Nd/144Nd signatures, and produced the relatively homogeneous 143Nd/144Nd composition that is characteristic of Réunion basalts. Our results show that Réunion magmas tap into a particularly ancient, primitive source compared with other volcanic hotspots, offering insight into the formation and preservation of ancient heterogeneities in Earth's interior.

Telltale tungsten and the Moon

Advances in high-precision isotopic analysis have provided key constraints on the origin and early evolution of the Earth and Moon. Measurements of the isotopes of tungsten provide the most stringent constraints on this history.

Accurate stable tungsten isotope measurements of natural samples using a 180W-183W double-spike

Tungsten is a moderately siderophile element and, thus, enriched in the Earth's core. Moreover, W behaves incompatibly during partial melting, causing relative enrichment in the Earth's crust compared to the mantle. However, little is known about the geochemical cycle of the redox-sensitive element W in the crust-mantle system and in modern to ancient low-temperature environments. High resolution stable W isotope measurements of rock samples from different geochemical reservoirs might be a powerful tool to better constrain this cycle. So far, low relative mass differences between the different W isotopes and analytical challenges hampered such high-resolution measurements. Notably, some pioneering studies on the stable W isotope composition of geological reference material show inconsistent results, calling for further verification of the true compositions of these materials.This study presents an analytical protocol for stable W isotope measurements including the calibration of a 180W-183W double-spike as well as W isotope and W concentration data of several geological reference materials (BHVO-2, AGV-2, SDC-1, W-2a, ScO-2, NOD-A-1, NOD-P-1). The reproducibility of stable W isotope measurements (±0.018‰ in δ186/184W; 2s.d.) is significantly improved compared to previous studies, which allows resolving between the stable W isotope compositions of various rock reservoirs on Earth. Relative to the NIST SRM 3163 standard, the highest δ186/184W value was observed for the Pacific Mn crust NOD-P-1 (+0.154±0.013‰; 2s.d.; n=6), which is significantly different from the δ186/184W value of the Atlantic Mn crust NOD-A-1 (+0.029±0.014‰; 2s.d.; n=6). Considering equilibrium fractionation between seawater WO42− and slowly growing Mn oxides, this indicates an isotopically heterogeneous distribution of W in the modern oceans. Igneous rocks also show a resolvable range in δ186/184W values. Magmatic reference materials range in δ186/184W between +0.016±0.032‰ (andesite AGV-2; 2s.d.; n=5) and +0.082±0.010‰ (basalt BHVO-2; 2s.d.; n=5) showing relative enrichment of light isotopes in more evolved magmatic rocks. These isotopic differences might result from isotope fractionation during magmatic differentiation. Alternatively, the mobilization of W by hydrothermal and/or magmatic fluids might be accompanied by isotope fractionation.

Modeling of nonstationary processes during separation of multicomponent isotope mixtures

ABSTRACTThe article presents a mathematical model for calculation of nonstationary hydraulic and separation processes in a gas centrifuge (GC) cascade for separation of multicomponent isotope mixtures. The model has been applied to calculate the parameters of nonstationary processes in a GC cascade for separation of krypton, germanium and tungsten isotopes. As a result, the specifics of the excess holdup distribution along the cascade stages has been identified, and variations of the isotope concentrations in a nonstationary process have been revealed. The data obtained show that the proposed mathematical model is able to adequately describe nonstationary hydraulic processes in GC cascades for separation of multicomponent isotope mixtures.Highlights:Mathematical model of cascade for separation of multicomponent isotope mixture has been developed.The model verification has been done.The isotope transient regularities into cascade during nonstationary processes has been identified.

Tungsten isotopes and the origin of the Moon

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 182W 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 182W compositions. Our results demonstrate that there are no resolvable radiogenic 182W 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 182W excesses, confirming that the Moon is characterized by a small, uniform ∼+26 parts-per-million excess in 182W 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 182W compositions. Mixing calculations demonstrate that this Earth–Moon 182W 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 182W excess in the Moon. Consequently, our results imply that post-giant impact processes might have modified 182W, leading to the similar 182W compositions of the pre-late veneer Earth's mantle and the Moon.

Meteorites formed in two reservoirs.

Cosmochemistry Meteorites are rocky debris left over from the formation of the solar system, which later fall to Earth. Kruijer et al. measured tungsten and molybdenum isotope ratios for a variety of iron meteorite groups and showed that they separate into two sequences—just like stony meteorites are already known to do. Because iron meteorites require parent bodies that grew massive enough to form metal cores, this dichotomy implies two separate regions in the early solar system where planetesimals formed. The authors speculate that the two reservoirs were respectively within and outside the orbit of Jupiter. If that is correct, the giant planet must have formed rapidly, before the meteorite parent bodies did. Proc. Natl. Acad. Sci. U.S.A. 10.1073/pnas.1704461114 (2017).

Jupiter is a big old planet

Jupiter is a case study in solar system superlatives. The gas giant is the biggest planet orbiting the sun, it’s the most massive, and new evidence suggests it’s also the oldest (Proc. Natl. Acad. Sci. USA 2017, DOI: 10.1073/pnas.1704461114). Using mass spectroscopy, researchers from Lawrence Livermore National Laboratory and the University of Munster observed that Earth’s iron meteorite samples cluster into two groups: those that are enriched in heavier isotopes of tungsten and molybdenum and those that aren’t. These data suggest that the solar system once had two distinct reservoirs where meteoric material amassed. Something must have kept these reservoirs separate, and a baby Jupiter, roughly 20 times the mass of Earth, is the likeliest explanation, say researchers led by Livermore’s Thomas S. Kruijer. On the basis of the ages of the dichotomous samples, the team posits that Jupiter’s birthday was about 1 million years after the formation of the

Beyond-mean-field effects on nuclear triaxiality

The beyond-mean-field effects on nuclear triaxiality are studied by applying the projected total energy surface (PTES) calculations to the light tungsten isotopes $^{170\text{--}178}\text{W}$, which have been well described as prolate rotors within the mean-field approximation. The present PTES calculations have well reproduced the experimental energies of the yrast states and the available experimental transition quardrupole moment (${Q}_{t}$) in function of spin. In particular, the results present a considerable large triaxiality for their ground states, with an average triaxial deformation $\ensuremath{\gamma}\ensuremath{\sim}{15}^{\ensuremath{\circ}}$. For a comparison, the total Routhian surface calculations have also been performed for these nuclei, the results show a well-established axial quadrupole deformation in their ground states. The presence of the significant triaxial deformation can be attributed to the beyond-mean-field effect as the angular momentum projection. This effect is therefore essential for a variety of mean-field approaches since it is only associated with the necessary restoration of the rotational symmetry in the laboratory frame, which is spontaneously broken in the intrinsic frame.

Systematic study of multi-quasiparticleK-isomeric bands in tungsten isotopes by the extended projected shell model

Background: The interplay between collective and single-particle degrees of freedom is an important structure aspect to study. The nuclei in theA ≈ 180 mass region are often denoted as good examples to study such problems because these nuclei are known to exhibit many rotational bands based on multi-quasiparticle K isomers. Purpose: A large set of high-quality experimental data on high-K isomeric states in the A ≈ 180 mass region has accumulated. A systematic description of them is a theoretical challenge as it requires a method going beyond the usual mean field with multi-quasiparticle configurations built in the shell-model basis. The K-isomer data provide an ideal testing ground for theoretical models. Method: The recently extended projected shell model (PSM) by the Pfaffian method is employed with a sufficiently large configuration space including up to 10 quasiparticles. The restoration of rotational symmetry which is broken in the deformed mean field is obtained by means of angular-momentum projection. With axial symmetry in the basis deformation, each multi-quasiparticle state, classified by a K quantum number, represents the major component of a rotational K band. Shell-model diagonalization in such a projected basis defines the K mixing, which is the key ingredient of the present method. Results: Quasiparticle structure and rotational properties of high-K isomers in even-even neutron-rich 174−186W isotopes are described. The rotational evolution of the yrast and near-yrast bands is discussed with successive band crossings. Multi-quasiparticle K isomers and associated rotational bands in each W isotope are studied with detailed quasiparticle configurations given. Electromagnetic transition properties are also studied and the calculated B(E2), B(M1), and g-factors are compared with experiment if data exist. Conclusions: Many nuclei of the A ≈ 180 mass region exhibit properties of an axially symmetric shape and K is approximately a good quantum number. For such nuclei, the extended PSM assuming an axially symmetric basis but including K mixing through diagonalization of the two-body Hamiltonian is an appropriate method to study multi-quasiparticle K isomers and K violations in these states. For special examples where one finds highly K-forbidden transitions the present model needs to be further improved.

Age of Jupiter inferred from the distinct genetics and formation times of meteorites

The age of Jupiter, the largest planet in our Solar System, is still unknown. Gas-giant planet formation likely involved the growth of large solid cores, followed by the accumulation of gas onto these cores. Thus, the gas-giant cores must have formed before dissipation of the solar nebula, which likely occurred within less than 10 My after Solar System formation. Although such rapid accretion of the gas-giant cores has successfully been modeled, until now it has not been possible to date their formation. Here, using molybdenum and tungsten isotope measurements on iron meteorites, we demonstrate that meteorites derive from two genetically distinct nebular reservoirs that coexisted and remained spatially separated between ∼1 My and ∼3-4 My after Solar System formation. The most plausible mechanism for this efficient separation is the formation of Jupiter, opening a gap in the disk and preventing the exchange of material between the two reservoirs. As such, our results indicate that Jupiter's core grew to ∼20 Earth masses within <1 My, followed by a more protracted growth to ∼50 Earth masses until at least ∼3-4 My after Solar System formation. Thus, Jupiter is the oldest planet of the Solar System, and its solid core formed well before the solar nebula gas dissipated, consistent with the core accretion model for giant planet formation.

Tungsten Isotopes in Planets.

The short-lived Hf-W isotope system has a wide range of important applications in cosmochemistry and geochemistry. The siderophile behavior of W, combined with the lithophile nature of Hf, makes the system uniquely useful as a chronometer of planetary accretion and differentiation. Tungsten isotopic data for meteorites show that the parent bodies of some differentiated meteorites accreted within 1 million years after Solar System formation. Melting and differentiation on these bodies took ~1-3 million years and was fueled by decay of 26Al. The timescale for accretion and core formation increases with planetary mass and is ~10 million years for Mars and >34 million years for Earth. The nearly identical 182W compositions for the mantles of the Moon and Earth are difficult to explain in current models for the formation of the Moon. Terrestrial samples with ages spanning ~4 billion years reveal small 182W variations within the silicate Earth, demonstrating that traces of Earth's earliest formative period have been preserved throughout Earth's history.

High Precision Tungsten Isotope Measurements by MC‐ICPMS

High Precision Tungsten Isotope Measurements by MC‐ICPMS