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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 91 records · Page 5

FPMS_XPeRT_INL_Poster

As nuclear energy expands and experimental programs increasingly rely on the facilities at Idaho National Laboratory (INL) for reactor and fuel testing, research capabilities must also expand to meet these demands. A new Fission Product Monitoring System (FPMS) has been deployed at the Advanced Test Reactor (ATR) at the Auxiliary Lead-out Experiment (ALE) House to support this expanding fuel testing mission. By tracking gaseous fission products releases from test fuel in near real-time, release rates, calculated from FPMS data, can be used to characterize the effectiveness of fuel cladding, especially for Tri-structural Isotropic (TRISO) fuel concepts. The new iteration of the FPMS supports up to 14 fission product monitors for online fission-product tracking via gamma-ray spectroscopy of the experiment’s effluent gas. Each monitor consists of a nominally 10% HPGe detector housed in a copper-lined lead shield with a warm gas trap. The new system features gamma-ray count rate information with a five-second temporal resolution and provides isotopic activity every five minutes, capable of resolving multiple overlapping fission product releases over a broad range of activities in near real-time. This work includes data from ATR cycle 175D data to demonstrate these capabilities. The hourly resolution data shows general trends and significant releases over the cycle, while the 5-minute resolution data allows for a more detailed examination of events due to unexpected particle releases.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

What can we learn from N 2 O isotope data? – Analytics, processes and modelling

The isotopic composition of nitrous oxide (N 2 O) provides useful information for evaluating N 2 O sources and budgets. Due to the co–occurrence of multiple N 2 O transformation pathways, it is, however, challenging to use isotopic information to quantify the contribution of distinct processes across variable spatiotemporal scales. Here, we present an overview of recent progress in N 2 O isotopic studies and provide suggestions for future research, mainly focusing on: analytical techniques; production and consumption processes; and interpretation and modelling approaches. Comparing isotope–ratio mass spectrometry (IRMS) with laser absorption spectroscopy (LAS), we conclude that IRMS is a precise technique for laboratory analysis of N 2 O isotopes, while LAS is more suitable for in situ/inline studies and offers advantages for site–specific analyses. When reviewing the link between the N 2 O isotopic composition and underlying mechanisms/processes, we find that, at the molecular scale, the specific enzymes and mechanisms involved determine isotopic fractionation effects. In contrast, at plot–to–global scales, mixing of N 2 O derived from different processes and their isotopic variability must be considered. We also find that dual isotope plots are effective for semi–quantitative attribution of co–occurring N 2 O production and reduction processes. More recently, process–based N 2 O isotopic models have been developed for natural abundance and 15 N–tracing studies, and have been shown to be effective, particularly for data with adequate temporal resolution. Here, despite the significant progress made over the last decade, there is still great need and potential for future work, including development of analytical techniques, reference materials and inter–laboratory comparisons, further exploration of N 2 O formation and destruction mechanisms, more observations across scales, and design and validation of interpretation and modelling approaches. Synthesizing all these efforts, we are confident that the N 2 O isotope community will continue to advance our understanding of N 2 O transformation processes in all spheres of the Earth, and in turn to gain improved constraints on regional and global budgets.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Using Median Point in Keeling Plot to Reduce the Uncertainty of the Isotopic Composition of Evapotranspiration

Abstract The isotopic composition of evapotranspirationδ ET is a crucial parameter in isotope-based evapotranspiration (ET) partitioning and moisture recycling studies. The Keeling plot method is the most prevalent method to calculateδ ET , though it contains large extrapolated uncertainties from the least squares regression. Traditional Keeling regression uses the mean point of individual measurements. Here, a modified Keeling plot framework was proposed using the median point of individual measurements. We tested theδ ET uncertainty using the mean point [σ ET (mean)] and median point [σ ET (median)]. Multiple resolutions of input and output data from six independent sites were used to test the performance of the two methods. Theσ ET (mean) would be greater thanσ ET (median) when the mean value of inverse vapor concentration () is greater than the median value of inverse vapor concentration []. When applying the filter ofr 2 > 0.8, around 70% ofσ ET (mean) was greater thanσ ET (median). This phenomenon might be due to the normality of the vapor concentrationC υ producing the asymmetric distribution of 1/C υ . The median method could perform significantly better than the mean method when inputting high-resolution measurements (e.g., 1 Hz) and when the water vapor concentrationC υ is relatively low. Compared to the mean method, applying the median method could on average reduce 6.88% of ET partitioning uncertainties and could on average reduce 9.00% of moisture recycling uncertainties. This study provided a new insight of the Keeling plot method and emphasized handling model output uncertainty from multiple perspectives instead of only from input parameters.

Meteorology & Atmospheric Sciences↗

An algebraic convolution formulation for multiple-scattering correction in small-angle neutron scattering

Multiple scattering in small-angle neutron scattering (SANS) redistributes spectral weight and distorts structural interpretation, particularly for thick or strongly scattering samples. We develop a finite-dimensional spectral desmearing framework that corrects multiple scattering without resorting to integral transforms or model-dependent extrapolation. The primary intensity is expanded in an orthonormal basis adapted to the isotropic transverse-momentum measure, under which convolution reduces to a recursive tensor contraction, allowing the Poisson-weighted multiple-scattering series to be evaluated directly in a finite-dimensional basis representation. This formulation yields a stable forward–inverse mapping between apparent and primary spectra. Numerical tests demonstrate convergence under repeated convolution and accurate recovery of the single-scattering intensity. Application to SANS measurements collected at multiple neutron facilities, including the Spallation Neutron Source, the High Flux Isotope Reactor, and the Institut Laue-Langevin, shows the quantitative reconstruction of the underlying primary spectrum across a wide range of transmission conditions, including strongly attenuating samples. Here, the method provides a stable, model-agnostic framework for multiple-scattering correction in SANS and enables consistent structural interpretation across instruments and scattering regimes.

Tung, Chi-Huan [Oak Ridge National Laboratory (ORN↗

Apatite geochemistry as a tool for understanding the petrogenesis of layered mafic-ultramafic rocks in the Bushveld Complex, South Africa

The sources of the magmas that formed the Rustenburg Layered Suite of the Bushveld Complex in South Africa remain debated, despite decades of research. Vertical and lateral variation in bulk rock and mineral separate Sr-Nd isotopic compositions, which generally indicate enriched sources, demonstrate that the layered sequence was formed by the emplacement of multiple batches of magma, crucially resulting in episodes of PGE-Cr-V mineralisation. The Lu-Hf isotope compositions of zircon are, however, at odds with the bulk rock Sr-Nd isotopic heterogeneity as they show near homogeneous compositions throughout the layered sequence (εHf (2.06 Ga) =−8). This lack of variation in Hf isotope composition has been attributed to deep, continental lithospheric mantle-related and/or crustal contamination of plume-derived Bushveld magmas. In this study, we analysed the major, trace element and Sr-Nd isotope geochemistry of apatite in the Rustenburg Layered Suite. Apatite occurs as an intercumulus mineral in the lowermost regions and a cumulus mineral in the uppermost regions of the layered sequence and can therefore be used to test existing models for the isotopic disequilibrium between bulk rock Sr-Nd and zircon Hf isotopic compositions. Apatite is largely chlorapatite in the lowermost regions and fluorapatite in the uppermost regions of the layered sequence. The Merensky Reef is unusual in that it comprises both chlorapatite and fluorapatite. Apatite throughout the layered sequence is generally unzoned and shows no evidence of late-stage alteration. Trace element data show that apatite is enriched in L/HREE, with common negative Eu-Sr anomalies. These trace element signatures are consistent with a magmatic origin for the apatite grains, with prior, or concurrent, plagioclase crystallization from the same melt. Variability in in situ Sr and Nd isotope compositions of apatite is recorded throughout the layered sequence with εNd (2.06 Ga) compositions varying between −2.5 and − 10.2 and initial 87 Sr/ 86 Sr compositions varying between 0.7079 and 0.7103 (for the Marikana dikes only). The variability in Sr-Nd isotope compositions of apatite is consistent with the bulk rock (and mineral separate) variation in Sr-Nd isotope compositions, suggesting apatite preserves primary magmatic compositions in the Rustenburg Layered Suite.

Apatite↗

Uranium Processing Signatures for Nuclear Forensics (NA22 End of FY23 Report)

A vacuum induction melting (VIM) furnace was used to produce an ~120 kg depleted uranium (DU) rod in November 2021 from well characterized feedstock to investigate the separation of thorium (Th) and protactinium (Pa) from uranium (U) during U metal casting and quantify the behavior of the 230 Th/ 234 U and 231 Pa/ 235 U radiochronometry systems. This work suggested that while 234 Th, measured by gamma spectrometry, appears to segregate to the top and surface of the rod, the concentration of 230 Th determined by isotope dilution mass spectrometry (IDMS) in drill turnings from multiple locations in the rod, including the hot top, is relatively consistent. To evaluate whether Th is potentially enriched at only the very outer surface of the cast DU rod relative to the bulk material in the cast rod, thin surface samples were collected from the cast DU rod. Locations sampled included the inner diameter (ID) and outer diameter (OD) of the bottom of the casting and the ID, OD, and top face of the hot top (very top of the casting). The locations are shown in Figure 1. Four samples were taken from each location at different depths in the cast material. Each cut took approximately 0.03 – 0.05” off of the casting.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Shape evolution in neutron-rich odd-even 105–109 Nb isotopes

Background: Neutron-rich nuclei around 𝑍 ≈ 40 are well known for exhibiting multiple shape transitions. Here, this region shows one of the sharpest shape transitions in the nuclear chart, evolving from a spherical vibrator at 𝑁 = 58 to a strongly deformed prolate shape at 𝑁 = 60. The largest deformations are observed for 38 Sr and 40 Zr . This abrupt shape transition disappears at 𝑍 = 36 and below, where a shape transition from spherical to oblate nuclei is predicted. On the other hand, for 𝑍 ≥ 42 and 𝑁 ≥ 60, the shape is known to evolve from axial to triaxial. While the even-𝑍 nuclei in this region have already been extensively studied, new insights can be gained from the studies of odd-𝑍 isotopes for a better understanding of the underlying mechanisms driving these phenomena. Purpose: The 41 Nb nuclei lie at the boundary between axially deformed Zr and triaxially deformed Mo nuclei. This work investigates the nuclear structure of very neutron-rich Nb nuclei up to 𝑁 = 68. The goal is to understand how the nuclear shape evolves as a function of isospin in this isotopic chain and provide new insights into the emergence of triaxial deformation. Methods: The structure of the neutron-rich Nb isotopes was investigated using state-of-the-art high-resolution 𝛾-ray spectroscopy of fission fragments produced via two different fission reactions. The use of 9 Be ⁢( 238 U, 𝑓) inverse kinematics, with a detection system comprising AGATA, EXOGAM, and VAMOS++, enabled the measurement of prompt and delayed 𝛾 rays from isotopically identified fission fragments, and 𝛾−𝛾−𝛾−𝛾 highfold data were obtained from a spontaneous fission source of 252 Cf using the Gammasphere array. Results: The level scheme of 105 Nb has been significantly extended, with the addition of two negative-parity bands observed for the first time. A new level scheme is proposed for 107 Nb, which is not in agreement with an earlier measurement, and new levels and transitions have been added to the very neutron-rich 109 Nb. The degree of triaxiality of the new bands is discussed on the basis of signature splitting analysis. The recently reported level scheme of 99 Nb has been revised. Conclusions: This systematic study on the Nb isotopic chain, compared to Zr and Mo, indicates that while the ground-state band exhibits a triaxial deformation, attributed to a proton hole coupled to a triaxially deformed Mo core, the negative-parity bands, based on isomeric bandheads, display an axially symmetric deformed structure, similar to that observed in the Zr isotopes, revealing the existence of a shape coexistence in the neutron-rich Nb nuclei.

Abushawish, M. [Université Claude-Bernard Lyon 1 (↗

Feasibility Study for Disposal Control Rod Assemblies Using UNF-ST&DARDS As-Loaded Zion Dual Purpose Cask Models

This report documents an initial evaluation to support future use of disposal control rod assemblies (DCRAs) for post-closure criticality control in dual purpose canisters (DPCs). The work described herein is an extension of previous efforts performed by Walker using inputs generated by the Used Nuclear Fuel-Storage, Transportation & Disposal Analysis Resource and Data System (UNFST&DARDS) for the Zion site DPCs with as-loaded isotopic compositions. The results of this analysis demonstrate that there are multiple pathways to using DCRA for post-closure criticality control. Various configurations of DCRA material, diameter, number of rods per DCRA, and number and location of DCRAs within a DPC were shown to be effective in varying degrees for the set of DPCs analyzed by Walker. Because of the variations in DPC as-loaded isotopic compositions considered in an array of DCRA parametric sweeps, it can be concluded that a DPC-specific methodology is feasible (i.e., a one-size-fits-all approach may not be needed). Instead, the utility program created for this work can be expanded to develop capabilities to provide DPC-specific DCRA arrangements to limit cost and weight and to allow for operational considerations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Nuclear Uncertainties Associated with the Nucleosynthesis in Ejecta of a Black Hole Accretion Disk

Abstract The simulation of heavy element nucleosynthesis requires input from yet-to-be-measured nuclear properties. The uncertainty in the values of these off-stability nuclear properties propagates to uncertainties in the predictions of elemental and isotopic abundances. However, for any given astrophysical explosion, there are many different trajectories, i.e., temperature and density histories, experienced by outflowing material, and thus different nuclear properties can come into play. We consider combined nucleosynthesis results from 460,000 trajectories from a black hole accretion disk and find the spread in elemental predictions due solely to unknown nuclear properties to be a factor of a few. We analyze this relative spread in model predictions due to nuclear variations and conclude that the uncertainties can be attributed to a combination of properties in a given region of the abundance pattern. We calculate a cross-correlation between mass changes and abundance changes to show how variations among the properties of participating nuclei may be explored. Our results provide further impetus for measurements of multiple quantities on individual short-lived neutron-rich isotopes at modern experimental facilities.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

In Situ Oxygen Isotope Determination in Serpentine Minerals by SIMS: Addressing Matrix Effects and Providing New Insights on Serpentinisation at Hole BA1B (Samail ophiolite, Oman)

The ability to constrain the petrogenesis of multiple serpentine generations recorded at the microscale is crucial for estimating the extent and conditions of modern versus fossil serpentinisation in ophiolites. To address matrix bias effects during oxygen isotope analysis by SIMS, we present the first investigation analysing antigorite in the compositional range Mg# = 77.5–99.5 mole %, using a CAMECA IMS–1280 secondary ion mass spectrometer. Spot–to–spot homogeneity is ≤ 0.5‰ (2s) for the new antigorite reference materials. The relative bias between antigorite reference materials with different Mg/Fe ratios is described by a second order polynomial, and a maximum difference in bias of ~ 1.8‰ was measured for Mg# ~ 78 to 100. We observed a bias up to ~ 1.0‰ between lizardite and antigorite attributed to their different crystal structure. Orientation effects up to ~ 1‰ were observed in chrysotile. The new analytical protocol allowed the identification of oxygen isotope zoning up to ~ 7‰ in serpentine minerals from two serpentinites recovered from an area of active serpentinisation in the Samail ophiolite. Furthermore in situ analysis is capable of resolving isotopic heterogeneity that may directly reflect changes in the physical and chemical conditions of multiple serpentinisation events in the Samail ophiolite.

47 OTHER INSTRUMENTATION↗

Image mapping for multiple charge state beams using a beam induced fluorescence profile monitors

Work continues on a minimally invasive, nitrogen fluorescence gas sheet at the Facility for Rare Isotope Beams (FRIB). A low density gas sheet may be used to observe the 2D transverse beam profile of high intensity, multiple charge state beams with minimal interference. Spatially and temporally correlated profiles are of particular interest in locations where there is significant charge state spread, such as the FRIB linac folding segments. A low-density gas sheet measurement system offers advantages for gas handling in nitrogen sensitive areas, however signal intensity is significantly lower than techniques using higher density gas sheets and jets. This work discusses measurement considerations for photon distributions generated by several spatially separated interaction points and design considerations for a high-sensitivity optics system for handling the expected low signal intensity.

Accelerator Physics↗

Machine Learning to Select Experiments Driven by Fundamental Science and Applications for Targeted Nuclear Data Improvement

This work describes a blueprint for a process that accelerates progress in science by quantitatively answering the following question: What is the optimal combination of fundamental-science and application-driven experiments to maximally reduce pertinent data uncertainties? Answering this question entails solving a high-dimensional and complex optimization problem that is best solved with advanced statistic techniques often classified as machine learning. We apply this process within the framework of nuclear data with the aim to select an experiment combination that will reduce uncertainties in 239 Pu nuclear data for neutron energies between 1 and 600 keV. In this field, fundamental-physics driven data, called differential, look at one nuclear physics observable at a time. They are contrasted to application-driven, integral, data where one or few resulting values inform a broad set of nuclear data across several nuclides and energies. The candidates for integral experiments are criticality measurements that were refined by a genetic algorithm to be maximally sensitive to 239 Pu fission cross sections in the desired energy range. Twenty-three candidate differential experiments were investigated and span multiple nuclear physics observables (e.g., total, capture cross sections) for isotopes appearing in the integral experiments. The optimal combination among these candidate experiments was investigated via generalized least squares fitting, augmented with Gaussian processes to ameliorate statistical irregularities in data, and the D-optimality criterion. The latter evaluates for each pair of candidates the joint reduction in uncertainties of all 12200 nuclear data appearing in the integral experiments compared to the knowledge we have from 168 past experiments, theory, and nuclear data. We chose as differential measurements those that investigate 63 Cu and 239 Pu total cross sections, based on D-optimality rank and feasibility constraints. Two integral (criticality) experiments were selected: An experiment with Al 2 ⁢O 3 and graphite interleaved with Pu and a thick Cu reflector explores 1–30 keV, while we target the 30–600 keV range with an experiment that swaps boron in place of graphite with a different geometry.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Fitting $\overline{ν}$ for Minor Pu Isotopes

After successful fitting of prompt ν for 235 U, 238 U, and 239 Pu(n,f) using CGMF, we have moved on to the minor plutonium isotopes. Minor isotopes pose a greater challenge both because there is less data available and we do not, by default, have parametrizations in CGMF already. Initially, we had planned to mitigate these challenges—and provide consistency within CGMF—by taking a stepped approach to the optimization. Continuing from the 239 Pu work, we would then fit 241Pu(n,f) $\overline{ν}$, where there is also a number of experimental measurements, keeping consistency between the parameters that are included in the calculation for 239 Pu and 241 Pu. With these parametrizations settled, we could consistently optimize 240 Pu(n,f) $\overline{ν}$. Following that step, we would move on to 242 Pu(n,f) (and increasing neutron number) and 238 Pu(n,f) (and decreasing neutron number). By including the fissioning systems in this manner, we should be able to minimize the unknown parameters in CGMF. We were also able to develop systematics for the CGMF input parameters along the Pu isotopic chain. However, after studies in the beginning of FY23, where we found reasonable agreement between CGMF and experimental prompt neutron multiplicities for 238−242 Pu, using a compound mass dependent parametrization from, and from discussions with I. Stetcu and P. Talou, we instead performed the evaluation of all five isotopes simultaneously. For all parameters in CGMF, they are either the same for each compound nucleus, or have a dependence on the compound mass. The details of these updates are given in. This report builds upon those details. In this short report, we first give an example of how we have updated CGMF to include 240 Pu(n,f) and 242 Pu(n,f), keeping consistency with the current 239 Pu and 241 Pu calculations, but without rigorous optimization (Sec. 2). Then, we will show in Section 3 what experimental data exist for the various isotopes to provide some insight into why 241 Pu and 239 Pu are used as anchor points. The evaluation is detailed in Section 4, and the comparison between CGMF calculations using the evaluated parameters and other prompt observables besides average neutron multiplicity are discussed in Section 2.2. Finally, we present conclusions and future work in Section 5.

07 ISOTOPE AND RADIATION SOURCES↗

Consistent Evaluation of the Prompt-fission Neutron Spectrum and Multiplicity for n+ 235,238 U and n+ 239 Pu

This report was written to satisfy a FY20 NCSP milestone on 235,238 U and 239 Pu. The milestone requires to “finalize a report assessing our methodology to evaluate prompt-fission neutron spectrum (PFNS) and multiplicity consistently”. More specifically, we study whether the code CGMF can reproduce ENDF/B-VIII.0 evaluated PFNS and average prompt-fission neutron multiplicities, $\bar{v}$, for 235,238 U and 239 Pu using one joint parameter set per isotope. If CGMF is shown to be able to reasonably reproduce ENDF/B-VIII.0 within its model-parameter space, this code could be used for future consistent evaluations of PFNS and $\bar{v}$. To answer this question, we explore here the parameter space of CGMF and its impact on calculated values and whether they are close to evaluated and experimental data. We also list experimental data that would enter a future evaluation and statistics method that could be used to obtain evaluated data and covariances. We conclude that values of $\bar{v}$ calculated by CGMF are reasonably close to ENDF/B-VIII.0 data, while more work on modeling the PFNS is needed (parameter optimization and model improvements) to reliably use it for evaluations.

07 ISOTOPE AND RADIATION SOURCES↗

Multiple shape coexistence near {sup 118}Sn: First 0+ 3 lifetime measurement

The intruder bands in Sn isotopes, built on the 2p-2h excitation across the Z = 50 proton shell gap, are well-known examples of shape coexistence near the neutron mid-shell region. Spectroscopic signatures for shape coexistence include enhanced E0 transitions between the 0+ band heads. However, the underlying shape coexistence and mixing has been unclear because lifetime information for the excited 0+ states was incomplete in 118Sn. We thus present here the first measurement of the 0+ 3 lifetime in 118Sn using the fast-timing technique following thermal-neutron capture. The observed enhancement in ρ2(E0;0+ 3 → 0+ 2 ) of 150(30) milliunits provides compelling indications for multiple shape coexistence in 118Sn. Additionally, three distinct shapes in 116,118,120Sn naturally emerged in theoretical calculations based on the quantum-number-projected generator coordinate method employing a relativistic energy density functional.

Wu, F.↗

SIMS Analysis of d18O and d13C of Carbonate Cements in Shale & Mudstone. Final report

This project has had two primary goals: 1) improving new technology for in situ microanalysis of stable isotope ratios by SIMS (secondary ion mass spectrometry) and 2) evaluating the importance of in situ analysis for studies of carbonate cements within shales of the Bakken Petroleum System. The systematic relations of stable isotope ratios provide an important tool to help resolve critical questions in geology. Stable isotope analysis of carbonate cements in shale constrain many topics of interest to DOE including: CO2 sequestration, climate change, and the genesis and quality of rock reservoirs for petroleum, natural gas, and water. However, this evidence is often preserved as fine-scale zonation, which is homogenized by conventional bulk analysis of powders. Recently, analysis of ultra-small spots in polished samples at the University of Wisconsin WiscSIMS Lab. has documented stable isotope zoning in carbonates and other diagenetic cements at smaller scales than previously possible. We have made detailed studies of oxygen and carbon isotope ratios in diagenetic cements from shales of the Bakken Formation from the Williston basin and elsewhere. The Bakken contains both reservoir and source rocks for petroleum. Hydrofracturing has greatly enhanced production of oil in these tight reservoirs. The sediments contain zoned carbonate cements with growth textures that record multiple events. The growth of carbonate (dolomite) cements has been proposed to control reservoir quality, but previous stable isotope studies of homogenized powders could not resolve individual generations of cement and this proposal remains untested. Our better characterization of the multiple growth zones in these carbonates will aid in understanding the genesis of these tight reservoirs and the production of unconventional oil and gas. This study has also developed SIMS standards for analysis of all compositions of Ca-Mg-Fe carbonate and selected Mn-carbonates and hydromagnesite. We have refined techniques for improved accuracy of SIMS stable isotope analysis, and for sub-1-micron spot sizes. We have established protocols for mapping and correlating sample analyses at micron-scale using QGIS software.

04 OIL SHALES AND TAR SANDS↗