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At least 19 records
All sourcesNASA NTRSDOE OSTI
NASA NTRS1980

Hafnium isotope variations in oceanic basalts

Hafnium isotope ratios generated by the beta(-) decay of Lu-176 are investigated in volcanic rocks derived from the suboceanic mantle. Hf-176/Hf-177 and Lu/Hf ratios were determined to precisions of 0.01-0.04% and 0.5%, respectively, by routine, low-blank chemistry. The Hf-176/Hf-177 ratio is found to be positively correlated with the Nd-143/Nd-144 ratio and negatively correlated with the Sr-87/Sr-86 and Pb-206/Pb-204 ratios, and to increase southwards along the Iceland-Reykjanes ridge traverse. An approximate bulk earth Hf-176/Hf-177 ratio of 0.28295 is inferred from the bulk earth Nd-143/Nd-144 ratio, which requires a bulk earth Lu/Hf ratio of 0.25, similar to the Juvinas eucrite. Midocean ridge basalts are shown to account for 60% of the range of Hf isotope ratios, and it is suggested that Lu-Hf fractionation is decoupled from Sm-Nd and Rb-Sr fractionation in very trace-element-depleted source regions as a result of partial melting.

Patchett, P. J.↗
DOE OSTI2012

Discovery of gallium, germanium, lutetium, and hafnium isotopes

Currently, twenty-eight gallium, thirty-one germanium, thirty-five lutetium, and thirty-six hafnium isotopes have been observed and the discovery of these isotopes is described here. For each isotope a brief synopsis of the first refereed publication, including the production and identification method, is presented.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2019

Hafnium Isotope Ratio Method for Enhanced Safeguards at Research Reactors

Pacific Northwest National Laboratory (PNNL) is developing a Hafnium (Hf)-based, enhanced safeguards measure for the verification of energy production in a research reactor. Historically, verification of nuclear reactor use has been based on extracting and measuring physical samples from non-fuel components of the reactor. The Hafnium Isotope Ratio Method for Enhanced Safeguards (HIRMES) provides a means of verifying reactor operation based upon measuring the changes in isotopic ratios in purpose-built coupons. The first activity is installing a purpose-built, integrated sample collection coupon containing hafnium which undergoes isotopic changes when irradiated in the reactor. The second activity is analysis of the isotopic changes of the irradiated coupon after removal of the coupon using the isotope ratio method (IRM). The energy, or plutonium production, in a fission reactor can be estimated using IRM by measuring and correlating stable isotope ratios in non-fuel reactor components using standard reactor modelling methods. This paper presents HIRMES, a technology intended to provide an inexpensive, accurate, and robust measurement capability for validating operator declarations at low-power research reactors. Deploying HIRMES in research reactors would provide the IAEA with an in-core reactor “odometer” on total energy production with higher accuracy than other methods. HIRMES could be integrated in new fuel or reactor core designs as part of a protocol that is simple to implement and minimizes effort required of the operator or inspector. This paper also discusses early demonstrations at U.S. research reactors to-date, which demonstrate HIRMES as a practical tool for independent verification of low-power research reactor utilization. Specifically, the measurement uncertainty during an irradiation campaign of 39766 MWh was 22 MWh, representing two hours at a 10 MW reactor for a total irradiation campaign over the course of approximately six months.

research reactor safeguards, isotope ratio method↗
DOE OSTI2013

ZIRCONIUM—HAFNIUM ISOTOPE EVIDENCE FROM METEORITES FOR THE DECOUPLED SYNTHESIS OF LIGHT AND HEAVY NEUTRON-RICH NUCLEI

Recent work based on analyses of meteorite and terrestrial whole-rock samples showed that the r- and s- process isotopes of Hf were homogeneously distributed throughout the inner solar system. We report new Hf isotope data for Calcium-Aluminum-rich inclusions (CAIs) of the CV3 carbonaceous chondrite Allende, and novel high-precision Zr isotope data for these CAIs and three carbonaceous chondrites (CM, CO, CK). Our Zr data reveal enrichments in the neutron-rich isotope {sup 96}Zr (≤1ε in {sup 96}Zr/{sup 90}Zr) for bulk chondrites and CAIs (∼2ε). Potential isotope effects due to incomplete sample dissolution, galactic and cosmic ray spallation, and the nuclear field shift are assessed and excluded, leading to the conclusion that the {sup 96}Zr isotope variations are of nucleosynthetic origin. The {sup 96}Zr enrichments are coupled with {sup 50}Ti excesses suggesting that both nuclides were produced in the same astrophysical environment. The same CAIs also exhibit deficits in r-process Hf isotopes, which provides strong evidence for a decoupling between the nucleosynthetic processes that produce the light (A ≤ 130) and heavy (A > 130) neutron-rich isotopes. We propose that the light neutron-capture isotopes largely formed in Type II supernovae (SNeII) with higher mass progenitors than the supernovae that produced the heavy r-process isotopes. In the context of our model, the light isotopes (e.g. {sup 96}Zr) are predominantly synthesized via charged-particle reactions in a high entropy wind environment, in which Hf isotopes are not produced. Collectively, our data indicates that CAIs sampled an excess of materials produced in a normal mass (12-25 M{sub ☉}) SNII.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2010

Discovery of Highly Excited Long-Lived Isomers in Neutron-Rich Hafnium and Tantalum Isotopes through Direct Mass Measurements

A study of cooled {sup 197}Au projectile-fragmentation products has been performed with a storage ring. This has enabled metastable nuclear excitations with energies up to 3 MeV, and half-lives extending to minutes or longer, to be identified in the neutron-rich nuclides {sup 183,184,186}Hf and {sup 186,187}Ta. The results support the prediction of a strongly favored isomer region near neutron number 116.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2015

Optimization of Hafnium dimensions for thermal epithermal experiments (TEX) with highly enriched uranium Jemima plates and polyethylene - 14517

The goal of the US Nuclear Criticality Safety Program's Thermal Epithermal experiments (TEX) is to design and conduct new critical experiments to address high priority nuclear data needs from the nuclear criticality safety and nuclear data communities, with special emphasis on intermediate energy (0.625 eV - 100 keV) assemblies. The second set of TEX experiments will use stacks of highly enriched uranium Jemima plates, hafnium (Hf) diluent plates, and polyethylene moderator plates to create assemblies that span a wide range of fission energy spectra, from thermal, through intermediate, to fast energies. As the hafnium plates need to be fabricated and represent a significant cost for this experiment, a parameter study examining experimental configurations with various Hf thicknesses was completed using KENO V.a to determine optimal dimensions. The Hf plate thicknesses were optimized based on three major design criteria: 1) ensuring thermal, intermediate, and fast critical configurations could be built, 2) creating assemblies with a height to diameter ratio of approximately one, and 3) maximizing sensitivity to hafnium isotope cross sections, as predicted by the SCALE/TSUNAMI package. Based on the calculations presented in this report, a hafnium thickness of 0.10 cm will result in compact critical assemblies using the existing Jemima plate inventory, while reducing Hf cost and ensuring adequate sensitivity of the system to hafnium cross sections. (authors)

42 ENGINEERING↗
DOE OSTI2021

Separation of zirconium and hafnium from early actinides and rare earth elements with eichrom’s pb resin in HCl

The separation of zirconium and hafnium isotopes from the early actinides and rare earth elements (REE) with Eichrom’s Pb resin has been studied. Batch studies were performed to characterize the behavior of actinium, thorium, zirconium, hafnium, lutetium, and yttrium on Pb resin from HCl solutions (0.001 M to 11 M). The early actinides and REE had no affinity for the resin at any concentration of HCl, but zirconium and hafnium showed a moderate uptake at high concentrations of HCl with a maximum extraction at 11 M HCl. Several column separations were tested, including with only tracer isotopes and with mass. Rapid, simple separations of zirconium from actinium, thorium, protactinium, and the REE with high yields and low elution volumes are presented with applications for tracer isotope production and fission product separations. Furthermore, the resin is less suitable for hafnium separations as hafnium tends to bleed off the resin even at high concentrations of HCl.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2010

Subduction Controls of Hf and Nd Isotopes in Lavas of the Aleutian Island Arc

The Hf and Nd isotopic compositions of 71 Quaternary lavas collected from locations along the full length of the Aleutian island arc are used to constrain the sources of Aleutian magmas and to provide insight into the geochemical behavior of Nd and Hf and related elements in the Aleutian subduction-magmatic system. Isotopic compositions of Aleutian lavas fall approximately at the center of, and form a trend parallel to, the terrestrial Hf-Nd isotopic array with {var_epsilon}{sub Hf} of +12.0 to +15.5 and {var_epsilon}{sub Nd} of +6.5 to +10.5. Basalts, andesites, and dacites within volcanic centers or in nearby volcanoes generally all have similar isotopic compositions, indicating that there is little measurable effect of crustal or other lithospheric assimilation within the volcanic plumbing systems of Aleutian volcanoes. Hafnium isotopic compositions have a clear pattern of along-arc increase that is continuous from the eastern-most locations near Cold Bay to Piip Seamount in the western-most part of the arc. This pattern is interpreted to reflect a westward decrease in the subducted sediment component present in Aleutian lavas, reflecting progressively lower rates of subduction westward as well as decreasing availability of trench sediment. Binary bulk mixing models (sediment + peridotite) demonstrate that 1-2% of the Hf in Aleutian lavas is derived from subducted sediment, indicating that Hf is mobilized out of the subducted sediment with an efficiency that is similar to that of Sr, Pb and Nd. Low published solubility for Hf and Nd in aqueous subduction fluids lead us to conclude that these elements are mobilized out of the subducted component and transferred to the mantle wedge as bulk sediment or as a silicate melt. Neodymium isotopes also generally increase from east to west, but the pattern is absent in the eastern third of the arc, where the sediment flux is high and increases from east to west, due to the presence of abundant terrigenous sediment in the trench east of the Amlia Fracture Zone, which is being subducting beneath the arc at Seguam Island. Mixing trends between mantle wedge and sediment end members become flatter in Hf-Nd isotope space at locations further west along the arc, indicating that the sediment end member in the west has either higher Nd/Hf or is more radiogenic in Hf compared to Nd. This pattern is interpreted to reflect an increase in pelagic clay relative to the terrigenous subducted sedimentary component westward along the arc. Results of this study imply that Hf does not behave as a conservative element in the Aleutian subduction system, as has been proposed for some other arcs.

58 GEOSCIENCES↗
DOE OSTI2026

Evidence for an isomeric {pi}½{sup +}[411] state in {sup 183}Ta

We report on the identification of a new isomeric state in Ta populated via the ground-state -decay of Hf. The experiment was performed at the KISS setup at RIKEN, where neutron-rich hafnium isotopes were produced via multi-nucleon transfer (MNT) reactions, followed by laser ionization of hafnium atoms, mass separation, and detection using an electron-gamma coincidence system. Isomeric spectroscopy was carried out by gating on different electron-gamma time correlations. A 459.1 keV -ray transition was identified in delayed spectra, and a half-life of μ was extracted through time-distribution fitting. The 459.1 keV state in Ta is known from previous work and has been assigned a Nilsson orbital configuration of , while a proposed new isomeric state above it is interpreted as a configuration that decays to via a low-energy, unobserved E2 transition. This is consistent with the systematic trends in neighbouring odd-A nuclei and transition rate calculations. Similar content being viewed by others

Doshi, S.↗
NASA NTRS2004

Lunar and Planetary Science XXXV: Terrestrial Planets: Building Blocks and Differentiation

The session "Terrestrial Planets: Building Blocks and Differentiation: included the following topics:Magnesium Isotopes in the Earth, Moon, Mars, and Pallasite Parent Body: High-Precision Analysis of Olivine by Laser-Ablation Multi-Collector ICPMS; Meteoritic Constraints on Collision Rates in the Primordial Asteroid Belt and Its Origin; New Constraints on the Origin of the Highly Siderophile Elements in the Earth's Upper Mantle; Further Lu-Hf and Sm-Nd Isotopic Data on Planetary Materials and Consequences for Planetary Differentiation; A Deep Lunar Magma Ocean Based on Neodymium, Strontium and Hafnium Isotope Mass Balance Partial Resetting on Hf-W System by Giant Impacts; On the Problem of Metal-Silicate Equilibration During Planet Formation: Significance for Hf-W Chronometry ; Solid Metal-Liquid Metal Partitioning of Pt, Re, and Os: The Effect of Carbon; Siderophile Element Abundances in Fe-S-Ni-O Melts Segregated from Partially Molten Ordinary Chondrite Under Dynamic Conditions; Activity Coefficients of Silicon in Iron-Nickel Alloys: Experimental Determination and Relevance for Planetary Differentiation; Reinvestigation of the Ni and Co Metal-Silicate Partitioning; Metal/Silicate Paritioning of P, Ga, and W at High Pressures and Temperatures: Dependence on Silicate Melt Composition; and Closure of the Fe-S-Si Liquid Miscibility Gap at High Pressure and Its Implications for Planetary Core Formation.

Source record↗
DOE OSTI2023

TEX-Hf: Integral Experiment Execution of Thermal/Epithermal eXperiments using Highly Enriched Uranium with Polyethylene and Hafnium (IER-532 CED-3b Report)

This report documents the experimental configurations and measurements for IER-532, Thermal/Epithermal eXperiments (TEX) with highly enriched uranium (HEU) fuel and interstitial hafnium (Hf), moderated and reflected by polyethylene. TEX-Hf is a variation of and based on the TEX-HEU (IER-297) design, with the inclusion of hafnium. These configurations provide integral experiments for validation of hafnium in the thermal, intermediate, and fast neutron energy regimes by maximizing the sensitivity in k eff to the hafnium isotope cross sections. The experiment campaign was completed over seven weeks during the end of FY22 and beginning of FY23 at the National Critical Experiments Research Center at the Nevada National Security Site. The campaign produced seven experimental configurations, four reproducibility measurements, and many additional dimensional measurements that will be of use to the future benchmark evaluation of this experiment and other experiments using the same HEU fuel. Table 1 summarizes the TEX-Hf experimental configurations, including their physical parameters, calculated fission fractions, and estimated excess reactivities.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2010

Nuclear Data Sheets for A=182

Nuclear spectroscopic information for known nuclides of mass number 182 (Lu,Hf,Ta,W,Re,Os,Ir,Pt,Au,Hg, Tl,Pb) with Z=71 to 82 and N=111 to 100 have been evaluated and presented together with adopted energies and J{pi} of levels in these nuclei. No excited state data are yet available for {sup 182}Lu, while only limited structure information is available for {sup 182}Pb and {sup 182}Tl. Rotational band structures are known for {sup 182}Hg and {sup 182}Au but spin-parity assignments remain largely tentative. The decays of {sup 182}Lu, {sup 182}Hg, {sup 182}Au and {sup 182}Tl are not well established. The {sup 182}Hf isotope is of geophysical and astrophysical interest. This evaluation supersedes previous full evaluations of A=182 published by 1988Fi05 and 1975Sc13, and a selected (mainly high-spin) update of A=182 published by 1995Si04.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2018

Neoproterozoic glacial origin of the Great Unconformity

The Great Unconformity, a profound gap in Earth’s stratigraphic record often evident below the base of the Cambrian system, has remained among the most enigmatic field observations in Earth science for over a century. While long associated directly or indirectly with the occurrence of the earliest complex animal fossils, a conclusive explanation for the formation and global extent of the Great Unconformity has remained elusive. In this paper, we show that the Great Unconformity is associated with a set of large global oxygen and hafnium isotope excursions in magmatic zircon that suggest a late Neoproterozoic crustal erosion and sediment subduction event of unprecedented scale. These excursions, the Great Unconformity, preservational irregularities in the terrestrial bolide impact record, and the first-order pattern of Phanerozoic sedimentation can together be explained by spatially heterogeneous Neoproterozoic glacial erosion totaling a global average of 3–5 vertical kilometers, along with the subsequent thermal and isostatic consequences of this erosion for global continental freeboard.

58 GEOSCIENCES↗
DOE OSTI2022

Development of Chemical Procedures for Isotope Harvesting: Separation of Trace Hafnium from Tungsten

The separation of trace hafnium from bulk tungsten alloys is of interest for isotope harvesting at the National Superconducting Cyclotron Laboratory and the Facility for Rare Ion Beams because 172 Hf, the parent of 172 Lu, accumulates in tungsten alloy beam blockers at these facilities. In this work, a procedure for the separation of trace hafnium from a bulk tungsten alloy (454 g) was established using tracer isotopes ( 175 Hf, 88 Zr, 173 Lu, and 88 Y). Here, the procedure employed dissolution in an HF–HNO 3 solution followed by a calcium fluoride precipitation, and then extraction chromatography was used for more selective separation steps. Two stages of column separations using LN resin (HDEHP based) and TRU resin (CMPO based) were performed. Gamma-ray spectroscopy and mass spectrometry were used to analyze the final hafnium sample and follow the steps in the chemical processing. Furthermore, the final recovery of hafnium was high (90 ± 8)%, and the mass of tungsten and other transition metals was reduced to near background levels (as determined by ICP-MS of the blank acid solutions). Zirconium follows hafnium quantitatively in this procedure; there was no detectable 173 Lu in the final hafnium sample.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2010

IRON-60 HETEROGENEITY AND INCOMPLETE ISOTOPE MIXING IN THE EARLY SOLAR SYSTEM

Short-lived radionuclides (e.g., {sup 26}Al, {sup 53}Mn, {sup 60}Fe, {sup 182}Hf) are widely used to refine the chronology of the early solar system. They provide chronological information, however, only if they were homogeneously distributed in the source region of the objects under scrutiny at the time of their formation. With the high level of precision now achieved on isotopic measurements, very short time intervals can in principle be resolved and a precise evaluation of the initial homogeneity degree becomes increasingly crucial. High-precision nickel isotope data for differentiated meteorites (angrites, ureilites) and chondritic (CB) components allow us to test the initial distribution of radioactive {sup 60}Fe and stable Ni isotopes. Although these meteorites appear to have formed nearly contemporaneously, they yield variable initial {sup 60}Fe/{sup 56}Fe ratios. Besides, the CB metal nodules and ureilite silicates show nucleosynthetic anomalies. The new data presented here do not confirm the recently inferred late injection of {sup 60}Fe into the protoplanetary disk. Instead, live {sup 60}Fe was present, but heterogeneously distributed, from the start of the solar system, revealing an incomplete mixing of material from various nucleosynthetic sources and restricting the use of the {sup 60}Fe-{sup 60}Ni system as a chronometer.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2016

From planetesimals to planets in turbulent protoplanetary disks. I. Onset of runaway growth

When planetesimals grow via collisions in a turbulent disk, stirring through density fluctuation caused by turbulence effectively increases the relative velocities between planetesimals, which suppresses the onset of runaway growth. We investigate the onset of runaway growth in a turbulent disk through simulations that calculate the mass and velocity evolution of planetesimals. When planetesimals are small, the average relative velocity between planetesimals, v{sub r}, is much greater than their surface escape velocity, v{sub esc}, so that runaway growth does not occur. As planetesimals become large via collisional growth, v{sub r} approaches v{sub esc}. When v{sub r}≈1.5v{sub esc}, runaway growth of the planetesimals occurs. During the oligarchic growth subsequent to runaway growth, a small number of planetary embryos produced via runaway growth become massive through collisions with planetesimals with radii of that at the onset of runaway growth, r{sub p,run}. We analytically derive r{sub p,run} as a function of the turbulent strength. Growing ∼10 M{sub ⊕} embryos that are suitable to become the cores of Jupiter and Saturn requires r{sub p,run}∼100 km, which is similar to the proposed fossil feature in the size distribution of main belt asteroids. In contrast, the formation of Mars as quickly as suggested from Hf-W isotope studies requires small planetesimals at the onset of runaway growth. Thus, the conditions required to form Mars, Jupiter, and Saturn and the size distribution of the main-belt asteroids indicate that the turbulence increased in amplitude relative to the sound speed with increasing distance from the young Sun.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2011

Quadrupole moment measurements for strongly deformed bands in {sup 171,172}Hf

A lifetime experiment, using the Doppler-shift attenuation method, has been performed at Gammasphere to measure the transition quadrupole moments Q{sub t} of strongly deformed bands in {sup 171}Hf and {sup 172}Hf. The measured value of Q{sub t} {approx} 9.5 e b for the band labeled ED in {sup 171}Hf strongly supports the recent suggestion that this sequence and several structures with similar properties in neighboring Hf isotopes are associated with a near-prolate shape with a deformation enhanced relative to that of normal deformed structures. The measured values of Q{sub t} {approx} 14 e b for the bands labeled SD1 and SD3 in {sup 172}Hf confirm that these sequences are associated with a prolate superdeformed shape, a property inferred in earlier work from other measured characteristics of the bands. Similar bands in {sup 173-175}Hf are also likely to be associated with superdeformed shapes. The observations are in contrast to predictions of cranking calculations performed with the ultimate cranker code.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗