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At least 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Neutron-rich calcium isotopes within realistic Gamow shell model calculations with continuum coupling

Based on the realistic nuclear force of the high-precision CD-Bonn potential, we have performed comprehensive calculations for neutron-rich calcium isotopes using the Gamow shell model (GSM) which includes resonance and continuum. The realistic GSM calculations produce well binding energies, one- and two-neutron separation energies, predicting that 57 Ca is the heaviest bound odd isotope and 70 Ca is the dripline nucleus. Resonant states are predicted, which provides useful information for future experiments on particle emissions in neutron-rich calcium isotopes. Shell evolutions in the calcium chain around neutron numbers $\textit{N}$ = 32, 34, and 40 are understood by calculating effective single-particle energies, the excitation energies of the first 2 + states and two-neutron separation energies. The calculations support shell closures at 52 Ca ($\textit{N}$ = 32) and 54 Ca ($\textit{N}$ = 34) but show a weakening of shell closure at 60 Ca ($\textit{N}$ = 40). Finally, the possible shell closure at 70 Ca ($\textit{N}$ = 50) is predicted.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
NASA NTRS1975

76535 - An old lunar rock

Measurements of Rb-Sr systematics, K-Ar gas retention ages, and the isotopic compositions of He, Ne, and Ar have been performed for lunar troctolite 76535. Other investigators have presented evidence that this important rock formed as a cumulate at depth, which would make it an important link in the early chronology of the moon. Rb-Sr data do not define an isochron. Total Ar-40/K ages of whole rock and plagioclase range from 4.40-4.54 b.y. The trapped Ne and Ar in 76535 cannot be uniquely characterized as either 'planetary derived' or solar wind derived, but appear to have characteristics of both. The data suggest that 76535 formed 4.3-4.6 b.y. ago, and the accumulation process and/or subsequent annealing may have incorporated excess noble gases. Separation of radiogenic parents and daughters with incomplete isotopic equilibration may also have occurred during cooling or during a subsequent 'event'.

Bogard, D. D.↗
NASA NTRS1985

Anorthositic oceanic crust in the Archean Earth

Ultrapure minerals separated from eclogite inclusions in kimberlites were analyzed for Sm, Nd, Sr, and oxygen isotopes and for major and trace elements. Clinopyroxene (cpx) and garnet (gnt) are the only primary mineral phases in these rocks, and mineral phases and their alteration products. The WR sub calc. is the reconstructed bulk composition excluding all the contamination influences. Two groups of eclogites: are distinguished: (1) type A Noritic-anorthositic eclogites; and (2) type B Ti-ferrogabbroic eclogites. The oxygen isotopes are primary mantle-derived features of these rocks and are not caused by posteruption processes, as they were measured on unaltered, clean mineral separates and show a correlation with REE pattern and Sr and Nd isotopes. It is suggested that the variation of the oxygen isotopes are caused by crustal-level fluid-rock interaction at relatively low temperature. It is shown that oxygen isotopes variation in MORB basalts caused by the hydrothermal system are in the same range as the observed oxygen isotope variation in eclogites. A model to explain the new set of data is proposed. It is thought that some of these eclogites might be emplaced into the upper lithosphere or lower crust at the time corresponding to their internal isochron age. The calculated WR composition was used to estimate model ages for these rocks.

Jagoutz, E.↗
DOE OSTI2024

Parallel-plate avalanche counters for heavy-ion beam tracking: History and mysteries

Despite being an old detector concept, position-sensitive parallel-plate avalanche counters (PPACs) remain widely used today for heavy-ion position and timing measurements. In modern rare isotope beam facilities and large-acceptance fragment separators, PPACs are used to characterize beam properties (diagnostics), facilitate beam delivery (tuning), and provide event-by-event beam tracking for particle identification (PID). Most popular particle localization methods in PPAC detectors are based on strip electrodes electrically connected to resistive-chain circuits or delay lines. More exotic systems include optical readouts based on recording electroluminescence light with high-granularity photodetector arrays or high-resolution resistive anode electrodes. PPACs with conventional resistive-chain or delay-line readouts achieve typical position and time resolutions of below 1 mm ( σ ) and around 150 ps ( σ ), respectively. In addition, delay-line systems are capable of counting rates above several hundred kHz for beam areas of a few millimeters square, and around 1 MHz for larger beam sizes. Resistive-chain readouts have limited rates of a few tens of kHz. A review of the operation principles and performance of PPAC detectors is presented in this paper. We will discuss decades-long experience building and operating PPACs developed at the National Superconducting Cyclotron Laboratory, and then refined at the Facility for Rare Isotope Beams (FRIB), mostly focusing on the delay-line readout technique (DLPPAC). We will also discuss problems that arise due to electric discharges at high rates and briefly describe ongoing developments at FRIB. Published by the American Physical Society 2024

Physics↗
DOE OSTI2021

Combination of DGA and LN Columns: A Versatile Option for Isotope Production and Purification at Oak Ridge National Laboratory

The chromatographic resins DGA and LN have been used sequentially to separate curium, californium, plutonium, and various fission products (FPs) to obtain products with a pure radioisotope or a radioelement with high isotopic purity. This 2-step combination of resins has found applications in the 252 Cf and 238 Pu campaigns performed at Oak Ridge National Laboratory. Experiments have been carried out in glove boxes, shielded caves, and hot cells, demonstrating that these resins are adequate and maintain their performance in highly radiolytic environments. We find that using these resins has led to the recovery of curium highly enriched (>95%) in 248 Cm, the clean separation of 251 Cf for the superheavy element research, and the recovery of 147 Pm from the FP stream obtained during the 238 Pu production campaign while demonstrating that the raffinate post DGA is essentially free of transuranic elements.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2024

Complete resolution across the neodymium/samarium isotopic envelope with a liquid sampling‐atmospheric pressure glow discharge — Orbitrap mass spectrometer

Rationale Nd and Sm isotope ratios play an important role in geological dating and as nuclear forensic signatures; however, the overlap of the respective 144, 148, 150 Nd/Sm isobars requires prior separations to be performed before analysis on typical MS platforms. The work presented here overcomes these isobaric interferences using ultrahigh‐mass resolution to alleviate interference without prior chemical separations. Methods A liquid sampling‐atmospheric pressure glow discharge ion source was coupled to a standard, QExactive Focus Orbitrap mass spectrometer, providing a mass resolution of ~80 k. A Spectroswiss FTMS booster X2 data acquisition package was used to collect extended transients, providing much higher mass resolution; ~230 k and ~600 k are employed here for Nd and Sm isotopes. Results While the standard Orbitrap resolution is far greater than typical “atomic” MS platforms, it was insufficient to alleviate all isobars. The use of a resolution of ~230 k resulted in baseline separation across the entire isotopic envelope for both Nd and Sm. Isotope ratios obtained from Nd:Sm mixtures using high‐resolution were equivalent to those found for individual‐element solutions, while isotope ratios obtained at a resolution of ~80 k (standard for the OEM data system) showed large deviations. Conclusions Use of ultrahigh‐resolution is an attractive alternative to extensive chemical separations to alleviate severe isobaric interferences. Sufficient mass resolution greatly reduces/eliminates the need for sample manipulations (separations) before analysis while reducing costs and total analysis times.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1991

s-process Ba, Nd, and Sm in presolar SiC from the Murchison meteorite

Ion microprobe isotopic measurements of Ba, Nd, and Sm in the K-series SiC size separates on which noble gas measurements were made by Lewis et al. (1990) are reported. All elements show isotopic abundance patterns characteristic for the s-process. The Ba-134/Ba-136 ratios are distinct from solar, indicating that s-Ba in SiC is different from that in the solar system. Ba-138/Ba-136 ratios decrease with grain size; if interpreted as being due to different neutron exposures, this trend is opposite of that shown by the Kr-86/Kr-82 ratios. Although other isotropic ratios for Ba and those for Nd and Sm differ in detail from theoretical predictions, the disagreements probably being due to uncertainties in the n-capture cross sections and simplifications in the models, the general agreement of the data with models of s-process nucleosynthesis support an AGB star origin for the relatively fine-grain SiC under consideration. Ba-136 in SiC is up to 85 percent pure s-process.

Zinner, Ernst↗
DOE OSTI2025

Design of an Out-Of-Pile Experimental Facility to Demonstrate the Feasibility of In Situ Thermal Conductivity Measurements of Nuclear Fuels Under Irradiation

There is substantial merit in quantifying nuclear fuel performance under irradiation. At Oak Ridge National Laboratory (ORNL), the MiniFuel irradiation platform has become the primary test vehicle for conducting separate-effects fuel performance irradiation experiments. The MiniFuel experiment is a passively controlled capsule design deployed in the High Flux Isotope Reactor (HFIR) through which fuel performance data is collected post-irradiation. Separate effects fuels irradiation capabilities are being expanded at ORNL by developing instrumented capsule designs that aim to capture fuel performance phenomena in-situ. One such capsule will specifically target fuel specimen thermal conductivity changes as a function of fuel burnup. Due to the complexity of making this measurement on nuclear fuel in-pile, this paper describes the necessary out-of-pile testing conducted on the thermal conductivity capsule (TCC) design. The measurement is ascertained via a thermopile system with heat transferred unidirectionally through a surrogate fuel specimen sandwiched between two conductive materials. The capsules investigated in this study are representative of the in-pile design, with the primary departure from irradiation conditions being the distribution of heat generation within the capsule. In the out-of-pile experiment, an external heater was used to drive heat through the conductive slug materials and into the specimen. This paper expounds the design of the out-of-pile experimental system and the thermal conductivity measurement technique. Predictive models used to determine the sensitivity of the measurement to variables governing thermal contact conductance between the specimen and slug materials and to predict experimental results are also described. Data from the out-of-pile experiment will be used to validate the readiness of the design for insertion into HFIR for irradiation.

Parker, Trevor [ORNL]↗
NASA NTRS1993

Nitrogen isotopic signatures in agglutinates from breccia 79035

Agglutinates in the size range 125-175 microns from regolith breccia 79035 are substantially depleted in N compared with bulk 79035. Isotopically, agglutinate N closely resembles that found previously in ilmenite separates. The minimum (delta)N-15 value found during stepwise pyrolysis of agglutinates is significantly heavier than that observed for bulk 79035. The major host phase for trapped N in 79035, and the host phase of the lightest isotopic component(s), remain unidentified.

Kerridge, John F.↗
DOE OSTI2024

Modeling and design of a separate effects irradiation test targeting fission gas release from Cr-doped UO 2

Fission gas release (FGR) from nuclear fuel during operation can diminish heat transfer properties across the pellet-cladding gap and increase the fuel rod internal pressure, thereby posing a concern to fuel reliability and safety during an accident. Enlarging the fuel grain size, which has been shown to improve fission gas retention, can be achieved by doping the fuel feedstock prior to sintering. In this work, the BISON fuel performance code was used to predict FGR from undoped and chromia-doped UO 2 (referred to as Cr-doped UO 2 ) fuel specimens with different grain sizes and across various temperatures. The BISON models identified the irradiation conditions for which FGR is most significant, and a separate effects irradiation experiment in the High Flux Isotope Reactor (HFIR) was then developed targeting those conditions. Further, the experiment leveraged the MiniFuel irradiation capability at Oak Ridge National Laboratory and consisted of 12 fuel specimens of varying grain size and Cr content. A coupling scheme between BISON FGR results and the ANSYS finite element thermal model used for experiment design was formulated to predict cumulative FGR from each fuel specimen based on expected irradiation temperature histories. The fuel samples were fabricated and characterized as a part of this work, and the fuel compositions modeled in BISON were representative of the specimens used in the experiment. This combined modeling and experimental effort aims to study the effect of fuel grain size and Cr content on FGR and to provide simulated BISON FGR results that can be used for future model validation activities.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Sensitivity analysis of thermal contact conductance modeling to inform MiniFuel irradiation capsule designs

The MiniFuel irradiation platform has been developed by Oak Ridge National Laboratory as a flexible, high-throughput separate effects testing capability within the High Flux Isotope Reactor (HFIR). Finite element thermal models are relied upon to design MiniFuel experiments to achieve a specific time-averaged irradiation temperature for experimental objectives. A previous study identified that uncertainty in the component heat generation rates and thermal contact conductance (TCC) model are the most significant contributors to predicted fuel temperature variance. To address both sources of uncertainty, this work performs sensitivity analysis on the TCC model to identify high-impact, high-uncertainty parameters that contribute to fuel temperature variance. The TCC model is analyzed in increasing detail, first using a standalone Python code, then again after coupling Python to the BISON fuel performance code. Furthermore, the parameters with the largest contributions to fuel temperature variance which can be reduced through design changes are identified as the initial subcapsule gas pressure, contact pressure between the fuel and dish, and the effective surface roughness of the interface. A set of design recommendations for future capsule designs has been established and applied to reduce the previously quantified average fuel temperature uncertainty ranges of ± 40 °C in the HFIR vertical experiment facilities (VXF) and ± 80 °C in the removable beryllium (RB) reflector to approximately ± 32 °C and ± 53 °C, respectively. This equates to a 21 % and 33 % reduction in the uncertainty range of the average fuel temperature for VXF and RB, respectively.

BISON↗
DOE OSTI2022

The need for speed – Burnup determination of spent nuclear fuel

Here we present the application of a novel analytical approach for high-speed evaluation of burn-up in spent nuclear fuel. This automated online separation–direct analysis method, which simultaneously measures the isotopic compositions and concentrations of Nd, Pu, and U using isotope dilution-inductively coupled plasma mass spectrometry, enables the determination of burnup in as little as 4.5 h per sample with expanded uncertainties as low as 1.2% using as little as 1µg of fuel. We compare the determined burn-up values, sample requirements, and analysis times with an ultra-high precision, in-house developed, methodology which employs multiple analytical techniques to measure the isotopic compositions and concentrations of Nd, Pu, and U yielding burn-up values with expanded uncertainties as low as 0.49% at the 95% confidence level, the lowest reported to date.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2026

Near-Real-Time Material Tracking: Combining Vis–NIR Spectroscopy with Flow Sensing for Accurate Nd(III) Quantification

A fiber-optic visible–near-infrared (vis–NIR) absorption spectroscopy and flow sensor system has been developed for near-real-time tracking of Nd mass in the effluent stream from a column in a fume hood. The approach leverages two unique data streams and a partial least-squares regression (PLSR) model trained on vis–NIR absorption spectra of Nd(III) (0–1.5 M) in 1 M HNO 3 . In-line volumetric flow rate and vis–NIR spectra are measured in sequence after a chromatography column. The time stamps from each data stream are then synchronized, which allows integrated volumes to be combined with Nd(III) molarities predicted by a PLSR model to accurately calculate the Nd mass flowing through the column. This integrated measurement provides instantaneous mass flow and accumulates these data over time to obtain the total mass processed. The methodology developed in this study contributes critical technical infrastructure to improve monitoring capabilities to support chemical separations and the production of strategic materials and isotopes.

Irvine, Sawyer B. [Oak Ridge National Laboratory (↗
DOE OSTI2021

Ab Initio Limits of Atomic Nuclei

We predict the limits of existence of atomic nuclei, the proton and neutron drip lines, from the light through medium-mass regions. Starting from a chiral two- and three-nucleon interaction with good saturation properties, we use the valence-space in-medium similarity renormalization group to calculate ground-state and separation energies from helium to iron, nearly 700 isotopes in total. Here, we use the available experimental data to quantify the theoretical uncertainties for our ab initio calculations towards the drip lines. Where the drip lines are known experimentally, our predictions are consistent within the estimated uncertainty. For the neutron-rich sodium to chromium isotopes, we provide predictions to be tested at rare-isotope beam facilities.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Specifications of FIPD Fission Gas Release Data

All fission gas release data stored in the Fuels Irradiation & Physics Database (FIPD) was originally measured using the Gas Assay, Sample and Recharge (GASR) System in the Hot Fuel Examination Facility (HFEF). It is therefore called GASR data in FIPD. During the measurement of a sample, such as an irradiated EBR-II fuel element/capsule, a pinhole-sized region near the top of the element plenum was melted by a laser. Plenum gas then expanded into a calibrated volume (note: in this document, “sample” and “capsule/element” are used interchangeably consistent with GASR documents in FIPD). The pressure rise in the volume was recorded. Helium backfilling and expansion was then performed to determine the sample (e.g., fuel element plenum) volume using Boyle’s Law and assuming ideal gas behavior at constant temperature. With the plenum volume and the recorded pressure rise, the sample (e.g., fuel element plenum) pressure was derived with assumption of ideal gas law behavior. The plenum volume and pressure as well as the cladding temperature during the measurement were collected (GASR data in FIPD). Other records associated with the fission gas release data include: raw GASR data records including volumes and post-puncture pressures of seal head/sealing head and manifold, calibration data, backfilling gas pressure data, and the data analysis records. A sample(s) of the fission gas released from the plenum was collected by the GASR system into sample bottles. The chemical and isotopic composition of the gas sample was analyzed separately from GASR data, and will be discussed in a separate specification. The plenum volume, pressure, and cladding temperature during the measurement are typically utilized to determine the number of moles of gas in the plenum. This quantity is often compared to the number of moles of gas generated by fission events. However, calculating these values and their associated uncertainty is beyond the scope of this document, as it necessitates additional assumptions. The most important document to understand the FIPD fission gas data is the GASR operational manual (title: Gas Assay, Sample and Recharge System (GASR) operation and maintenance manual, HFEF/N OMM 4381, DOC. NO. W0018-0032-ES-00). This manual provides: (1) description of the GASR and the functions of each component (laser drilling, welding, seal head/sealing head, manifold, vacuum system, sample system, purge and gas tag system, etc.); (2) step-by-step guidance on calibrations, operations, and measurements; and (3) maintenance procedures and other details relating to the structure and operation of the GASR. Note that the original GASR operated until 2020. A new GASR with the same design and measurement methodology was installed in 2021. The specifications of the GASR presented on the HFEF website at this time are consistent with the ones given in the operational manual. The methods to calculate the plenum volume and pressures were not included in the operational manual, but were recorded in the legacy data analysis files. Details of the methods are given in Chapter 3.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1973

Extinct lunar radio activities - Xenon from Pu-244 and I-129 in Apollo 14 breccias.

Two Apollo 14 breccias have been found to contain xenon from the spontaneous fission of 82 my Pu-244. A third contains 60 times as much fission xenon as local uranium can account for and is probably of similar character. One of the breccias shows a Xe-129 excess most likely due to the decay of 17 my I-129. That these components can be separated and identified at all implies that complete isotopic homogenization has not occurred over a period which encompasses both extinction of these radionuclides and compaction of the breccias into their final form. In this sense isotope pre-history has been preserved in some lunar breccias providing information that pre-dates the formation of the rock itself (as determined by conventional techniques).

Behrmann, C. J.↗
NASA NTRS1979

Lead isotope systematics of three Apollo 17 mare basalts

The paper deals with new and more accurate determinations of uranium, thorium, and isotopic lead data for five bulk samples and separate pyroxene, ilmenite, and plagioclase from basalt 71055. In a concordia diagram, the samples suggest a postcrystallization disturbance of the U-Pb systems of the rock. There is no compelling reason, from U-Pb data, to believe that the moon is younger than 4.55 AE.

Tilton, G. R.↗
NASA NTRS1992

Rhenium in seawater - Confirmation of generally conservative behavior

A depth profile of the concentration of Re was measured in the Pacific Ocean using a technique developed for the clean chemical separation and the precise measurement of Re by isotope dilution and negative thermal ionization mass spectrometry (ID-NTIMS). We obtain a narrow range for Re from 7.20 +/- 0.03 to 7.38 +/- 0.03 ng/kg for depths between 45 m and 4700 m. This demonstrates that Re is relatively well mixed throughout the water column and confirms the theoretical prediction that the behavior of Re in the oceans is conservative. When examined in detail, both salinity and the concentration of Re increase by approximately 1.5 percent between 400 and 4700 m, a correlation consistent with conservative behavior. However, Re appears to be depleted relative to salinity by 1.0-1.5 percent at 100 m, and enriched by approximately 4 percent at the surface. These observations suggest a minor level of Re scavenging in near surface waters, and an input of Re to the ocean surface. This work demonstrates the utility of geochemical investigations of certain trace elements not previously been amenable to detailed study.

Anbar, A. D.↗