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At least 19 records

A new method for quantifying 64 Cu in nuclear debris samples

Quantifying 64 Cu in post-detonation nuclear debris samples can provide important diagnostic information regarding the structural materials used within a nuclear device. However, this task is challenging due to the weak gamma emissions associated with the decay of 64 Cu, its short half-life (12.701 h), and the presence of interfering fission product radioisotopes. Large quantities of debris sample are generally needed to accurately quantify 64 Cu, which can be problematic in sample-limited scenarios where other radiometric analyses are required. Herein, we present a new method for the separation of 64 Cu from solutions of mixed fission products and demonstrate the quantification of its activity through use of gas-flow proportional beta counting. Here, the new method was validated through a series of rigorous tests and was shown to improve the detection limit of 64 Cu by over two orders of magnitude, from 2.5 × 10 6 to 1.3 × 10 4 atoms/sample for 100 min measurements.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Exploring 𝛽 decay and 𝛽-delayed neutron emission in exotic 46,47 Cl isotopes

In this paper, 𝛽 − and 𝛽-delayed neutron decays of 46,47 Cl are reported from an experiment carried out at the National Superconducting Cyclotron Laboratory using the Beta Counting System. The half-lives of both 46 Cl and 47 Cl were extracted. Based on the delayed 𝛾-ray transitions observed, the level structure of 𝑁=28 46 Ar was determined. Completely different sets of excited states above the first 2 + state in 46 Ar were populated in the 46 Cl 𝛽⁢0⁢𝑛 and 47 Cl 𝛽⁢1⁢𝑛 decay channels. Two new 𝛾-ray transitions in 47 Ar were identified from the very weak 47 Cl 𝛽⁢0⁢𝑛 decay. Furthermore, 46 Cl 𝛽⁢1⁢𝑛 and 47 Cl 𝛽⁢2⁢𝑛 were also observed to yield different population patterns for levels in 45 Ar, including states of different parities. Here, the experimental results allow us to address some of the open questions related to the delayed neutron emission process. For isotopes with large neutron excess and high 𝑄 𝛽 values, delayed neutron emission remains an important decay mode and can be utilized as a powerful spectroscopic tool. Experimental results were compared with shell-model calculations using the FSU and 𝑉 MU effective interactions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Separation of rare earth element radioisotopes by reverse-phase high-speed counter-current chromatography

Analytical scale purification of rare earth element (REE) radioisotopes is typically accomplished using cation-exchange resins (e.g. AG 50W-X8) and high-performance liquid chromatography (HPLC). Despite the variety of improvements made since the development of this separation process in the 1950s, nearest neighbor separations remain a challenge, as does the issue of irreversible sample adsorption. Herein, we report a study that evaluates the potential of high-speed counter-current chromatography (HSCCC) as an alternative method for purifying REE elements, with specific reference to separations of fission product REE of interest to nuclear forensics. Complementary HSCCC REE separation experiments, one spiked with radiotracer and REE fission product activity, allowed for in depth analysis of resulting fractions from both an elemental (inductively coupled plasma atomic emission spectroscopy, ICP-AES) and radiological (gamma-ray spectrometry, beta counting) purity perspective. The highly reproducible nature of separation profiles generated from HSCCC instruments was leveraged to simplify work-up of samples containing radioisotopes. Subsequent radioanalytical evaluation revealed minimal carryover of Eu into neighboring Sm and Tb fractions (as indicated by presence of 150Eu), and trace contamination of the Tb fraction with Y (as indicated by presence of 91Y). Subtle differences in stationary phase retention across the two columns were reflected in significant variations in decontamination factors of duplicate parallel separations. Furthermore, these differences paired with obtained distribution of radioisotopes provided valuable insights into future improvements. Collectively, this study represents a significant step forward in development of HSCCC technology for task specific REE radioisotope purification.

07 ISOTOPE AND RADIATION SOURCES↗

Low spin spectroscopy of neutron-rich Cl 43 , 44 , 45 via β - and β n decay

In this article, β - decay studies of neutron-rich isotopes 43,45 S performed at the National Superconducting Cyclotron Laboratory are reported. β -delayed $\gamma$ transitions were detected by an array of 16 clover detectors surrounding the Beta Counting Station, which consists of a 40×40 double-sided silicon strip detector followed by a single-sided silicon strip detector. β -decay half-lives were extracted for 43,45 S by correlating implants and decays in the pixelated implant detector and by considering further coincidences with $\gamma$ transitions in the daughter nuclei. Further, the level structures of 43,45 Cl are expanded by the addition of 20 and 8 new $\gamma$ transitions in 43 Cl and 45 Cl respectively, and core-excited negative-parity states were observed in both nuclei for the first time. For 45 S, a large fraction of the β -decay strength was observed feeding neutron-unbound states in 45 Cl, which, decaying by delayed neutrons, populated excited states in the β ⁢1⁢ n daughter, 44 Cl. Experimental observations were compared to detailed shell-model calculations using the SDPFSDG-MU interaction to highlight the role of the diminished N = 28 neutron shell gap and the near degeneracy of the proton s 1/2 and d 3/2 orbitals in the structure of the neutron-rich Cl isotopes. The current work also provides further support to a ground-state spin-parity assignment of 3/2 + in 45 Cl.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

β -delayed neutron emission of Mn 64 , Cr 62 , and Fe 65

The β-decay properties of nuclei near the second nuclear “island of inversion” around neutron rich nuclei with neutron number 40 are important tests of nuclear structure models and interactions. In particular, the β-delayed neutron emission branch (Ρ n ), is useful for investigating β-strength and neutron-γ competition above the neutron separation energies of the daughter nuclei. We report new constraints for Ρ n values for three nuclei in the region: 62 Cr (Ρ n <1%), 64 Mn (Ρ n = 1.5⁢(6)%), and 65 Fe (Ρ n < 1%), measured with the Neutron Emission Ratio Observer (NERO) neutron long counter system and the Beta Counting Station (BCS) at the National Superconducting Cyclotron Laboratory (NSCL). Our results resolve the large discrepancy between previous direct and indirect measurements for 64 Mn and confirm the predictions of global theoretical models when a statistical treatment of the γ and neutron decays of the daughter states is included. Here we also obtain improved half-lives for 62 Cr [206(5) ms] and the short-lived isomer in the 62 Fe daughter [112(7) ms] from β-delayed γ emission data obtained in the same experiment with the Summing NaI (SuN) total absorption spectrometer. Finally, we use γ emission data to obtain a new upper limit for the 62 Cr β-decay population of the long-lived isomeric state in 62 Mn.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Local Power Impact Experiment Design for a New Fuel Type for use in the Advanced Test Reactor

The Advanced Test Reactor (ATR), and complimentary zero-power ATR Critical (ATRC) reactor, located at Idaho National Labs (INL), are undergoing conversion from Highly Enriched Uranium (HEU) to Low Enriched Uranium (LEU). Both have a variety of testing locations that can receive large variations in flux due to its unique serpentine design, consisting of five lobes (see Figure 1). Initial criticality and power distribution throughout the core are controlled by core-external outer shim control cylinders (OSCCs). Distinct test loops allow for testing at specific temperatures, pressures, and irradiation conditions. The ATR is one of the key nuclear engineering research and testing facilities within the DOE National Laboratory Complex, and the ATRC supports its operation [1]. Currently, the Office of Material Management and Minimization (M3) within the National Nuclear Security Administration of the DOE is working to convert the remaining research reactors, including the ATR, from 93% HEU fuel to 19.75% LEU fuel (LEU) to support non-proliferation [2]. Extensive materials testing at INL and internationally has demonstrated that a high-density uranium molybdenum (U 10Mo) alloy can meet the performance requirements of the remaining high powered research reactors. However, there are many technical challenges to address before the conversion to LEU can be successful, including the accurate characterization of the reactor core physics with LEU fuel. Reactor physics safety evaluations currently use Monte Carlo for the 21st Century (MC21), a continuous-energy Monte Carlo radiation transport code [3]. Existing MC21 models of the ATR and ATRC cores have a validation basis for use in neutronics analyses with HEU fuel. The models are used to support safety analyses that include comparisons to the safety requirements for the reactors. However, the use of the LOWE element in the ATR and ATRC is not currently covered by the current model validation basis. To deploy the new fuel type, extensive computational reactor physics support is necessary to support the use of LOWE in the ATR and ATRC. Therefore, LOWE requires a rigorous validation basis, aligned with that of HEU fuel, that takes advantage of the existing software tools and processes currently used for the ATR and ATRC. The experiment to validate of the MC21 models for determining power, the Power Impact Validation Experiment, will consist of two flux runs in the ATRC, one with fully HEU loading and one with a single LOWE element. Both flux runs will be instrumented with 20 sets of azimuthal fission wires and 3 sets of axial fission wires, as shown in Figure 4. Standard flux run methodology will be used [4]. Power Impact Validation Experiment data will be compared against MC21 calculated data, both for absolute fission rate accuracy and to determine the relative change in fission rates between the two runs. The results of the Power Impact Validation Experiment and subsequent evaluations will provide the validation basis for MC21 for use with LOWE elements. Key features of the Power Impact Validation Experiment include: (1) Two flux runs to allow for LOWE perturbed measurements to be compared to already validated measurements taken from a full core of HEU fuel, (2) Optimization of instrumentation to balance analytical needs with practical considerations (e.g., limited time window to count beta particles from fission products), and (3) Standard ATRC core loading, including both driver positions and flux traps, to minimize cost while remaining representative of typical ATR core loading.

42 ENGINEERING↗

Radioisotope dating of nuclear materials using cryogenic decay energy spectrometry

Cryogenic decay energy spectrometry provides high energy resolution and enables absolute decay counting, offering an alternative measurement technique for radiochronometry. A cryogenic decay energy spectrometry experiment was conducted using a magnetic microcalorimeter to determine the age of a plutonium sample. The energy resolution was measured at 0.05% from 5 to 6 MeV. The time since sample purification was determined using the measured concentration ratio of the 241 Am/ 241 Pu radiochronometer. Sample age estimates based on 241 Pu alpha-decay and beta-decay counts, along with 241 Am decay counts, align with the expected sample age within expanded uncertainty (k = 2), supporting the accuracy of cryogenic decay energy spectrometry as a radiochronometric method.

and nuclear chemistry↗

147 Nd Quantification Using HSCCC-Purified Samples

Quantifying the fission product 147 Nd in nuclear debris samples is an important component of post-detonation nuclear forensics. The most accurate quantifications are obtained when Nd is purified from all other fission products, actinides, activation products, and environmental matrix contained within the debris. In this study, a recently developed method for Nd purification was tested, purifying 147 Nd from solutions of mixed fission products using high-speed counter-current chromatography (HSCCC). Importantly, the new method allowed for faster elution of Nd from the column as compared with established high performance liquid chromatography (HPLC) methods, and resulted in accurate/precise 147 Nd quantification by gamma-ray spectrometry. While the up-front equipment costs associated with HSCCC may be higher, its operational costs are on par with those of HPLC (solvents, extractants, power). Gas-flow proportional beta decay counting revealed contamination from the nearest neighbor lanthanide 143 Pr (a gamma-silent radioisotope) in the HSCCC-purified samples, but the activity contribution from 147 Nd could still be quantified. Remarkably consistent elution profiles were observed for the HSCCC method, spanning rare earth element (REE) loadings of more than 10 orders of magnitude (tracer to mmol quantities). In conclusion, the reliability and speed of the new method suggest utility for the rapid separation and quantification of 147 Nd in unknown samples.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

127 Xe quantification method development and intercomparison exercise

Monitoring of the atmosphere for fission products ( 131m Xe, 133m Xe, 133 Xe, and 135 Xe) is performed by various laboratories to detect nuclear explosions. Quantification of 127 Xe is not routinely performed by laboratories measuring atmospheric radioxenon because it is not a fission product. 127 Xe was recently detected by a ground-based beta-gamma air monitoring system. When measured using beta-gamma coincidence detector systems, such as those in use on the International Monitoring System (IMS) of the Comprehensive Nuclear-Test-Ban Treaty (CTBT), 127 Xe can interfere with the quantification of fission product radioxenon due to overlap of the 127 Xe beta-gamma coincidence signatures with those of fission product radioxenon. Here, this work demonstrates quantification of 127 Xe at different laboratories with different measurement techniques. Production and purification of 127 Xe was performed by neutron activation of enriched 126 Xe. The purified 127 Xe was then split between laboratories, and detection and quantification methods were developed. At Idaho National Laboratory, a quantification method involving high purity germanium detectors was devised that included self-attenuation correction. At AWE, a beta-gamma coincidence counting method, as used in support of the IMS, was modified to enable the measurement and analysis of the 127 Xe samples. Corrections were made for self-attenuation, which showed a strong xenon volume dependency, for some coincidence signatures. The gas sample activity concentration was used as the comparison metric and it showed excellent agreement between the methods.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Deployment of portable, modular gas samplers as part of an atmospheric tracer experiment

Underground nuclear explosions release noble gases into the atmosphere that can be detected to support international monitoring efforts. Atmospheric transport models help predict the movement of these gases over long distances, but struggle to predict the movement in the atmosphere local to the release. A field experiment was designed to monitor the movement of 127 Xe within a 5-km radius. Four gas samplers were deployed as part of this experiment to collect atmospheric samples at various distances from the release point. In conclusion, these samples were then analyzed in a near-field lab using a NaI detector and in an off-site lab using gamma-gamma coincidence and beta-gamma coincidence counting.

Radioxenon↗

A Short-Lived Isotope Counting System (SLICS) to measure reaction cross sections producing light, beta-decaying nuclei on OMEGA

A new activation detector optimized for short-lived isotopes was designed, installed, and tested on OMEGA. The Short-Lived Isotope Counting System (SLICS) can be positioned as close as 35 cm from the OMEGA target chamber center in a ten-inch-manipulator. Stable target samples can be mounted on the front end of the detector assembly to undergo triton-, deuteron-, or neutron-induced reactions that produce short-lived reaction products that beta decay. The emitted betas are detected in a phoswich configuration to eliminate the gamma background. The detector is optimized for isotopes with half-lives from 150 ms to 20 s, filling a gap in OMEGA’s current activation detectors for isotopes with half-lives >5 min. In a pilot study, SLICS achieved an efficiency of 24.5% ± 2.0% for counting 8Li, with a total of 505.8 ± 4.4 qualifying events. Using the existing triton laser-ion acceleration platform on OMEGA, this detector can be used to measure rarely studied tritium-induced reactions on light nuclei with an estimated uncertainty of 12%. As a result, the design of the detector and its performance during a first experiment employing deuterium as a surrogate will be discussed.

Beta spectrometry↗

Integrating Metal-Hydride and Gas-Detector for Tritium Gas Detection

Detection of trace amounts of environmental tritium is a challenging problem, driving the need for field-deployable systems that offer high sensitivity, selectivity, and minimal false positives. We present a technique for high-sensitivity, high-selectivity tritium measurement, which integrates metal-hydride and gas-detector concepts into a compact field-deployable tritium sensor. A hydrogen-storage metal embedded in a gas proportional counter selectively absorbs protium (1H)/tritium (3H), which are subsequently released into the counter volume with a reduced radiation background. Ionizations induced by 3H beta particles are then measured in proportional counting mode, achieving high detection efficiency. Preliminary studies conducted with palladium (Pd) thin films coated on stainless-steel substrates demonstrated 3H absorption and metal-tritide formation, followed by 3H desorption upon heating the metal-tritide. These processes were confirmed using activity concentrations measured by a commercial tritium monitor and pulse height spectra acquired from a custom-built detector.

Gas-proportional counter↗

Generalized eikonal identities for charged currents

Abstract We discuss QED radiative corrections to contact operators coupling two heavy fields and one light field. These operators appear ubiquitously in weak interactions with nuclei such as beta decay and neutrino nucleus scattering. New eikonal identities are derived in the static limit (i.e., neglecting nuclear recoil) that allow for manifest power counting of enhancements proportional to the charge of the nucleus. We apply these new identities to nuclear beta decays and find that the “independent particle model” used by Jaus, Rasche, Sirlin & Zucchini is closely related, though not identical, to a model independent effective field theorcalculation.

Physics↗

Multiple Changepoint Detection for Non‐Gaussian Time Series

ABSTRACT This article combines methods from existing techniques to identify multiple changepoints in non‐Gaussian autocorrelated time series. A transformation is used to convert a Gaussian series into a non‐Gaussian series, enabling penalized likelihood methods to handle non‐Gaussian scenarios. When the marginal distribution of the data is continuous, the methods essentially reduce to the change of variables formula for probability densities. When the marginal distribution is count‐oriented, Hermite expansions and particle filtering techniques are used to quantify the scenario. Simulations demonstrating the efficacy of the methods are given and two data sets are analyzed: 1) the proportion of home runs hit by Major League Baseball batters from 1920 to 2023 and 2) a six‐dimensional series of tropical cyclone counts from the Earth's basins of generation from 1980 to 2023. In the first series, beta marginal distributions are used to describe the proportions; in the second, Poisson marginal distributions seem appropriate.

Lund, Robert [Department of Statistics University ↗

Online Alpha Monitoring of High Cs-137 Hanford and SRS High Level Waste with Tensioned Metastable Fluid Detectors

The Department of Energy’s Hanford and Savannah River Sites maintain millions of gallons of caustic supernate and salt high activity waste in their high-level waste (HLW) tank farm inventories. The Savannah River Site is currently treating this waste with a calixarene-based solvent extraction of Cs-137 to reduce these inventories. Hanford is employing an at-tank crystalline silico titanate (CST) based solid phase extraction methodology to reduce their liquid HLW inventories. Due to the high solubility of Cs-137 and the relative insolubility of the actinides in these caustic waste forms, the beta to alpha radioactivity ratio can often exceed six orders of magnitude in the feed solutions to these treatment processes. This unique characteristic leads to significant technical challenges in making rapid gross alpha measurements in the presence of the overwhelming beta, gamma, as well as dissolved sodium salt in these HLW matrices. Conventional radioanalytical techniques, such as liquid scintillation analysis or gas flow proportional counting require significant radiochemistry preparation prior to the radiometric measurements for gross alpha activity. These required pretreatments render these technologies untenable for rapid quantification of gross alpha activity that could be required to support on or at-line measurements ensuring a waste stream will meet regulatory requirements. The radiation measurement properties of Tensioned Metastable Fluid Detectors (TMFDs) have been studied by Purdue University’s Taleyarkhan research group for well over a decade. Fluids tensioned to the appropriate degree will rupture when struck by radiation, resulting in a measurable cavitation event. The negative pressure generating this tension can be adjusted by centrifugal rotation or by acoustic means in such a way that these cavitation events can be generated from alpha radiation but will not be generated by beta or gamma radiation. Purdue University and the Savannah River National Laboratory are currently collaborating to develop a gamma/beta blind, spectroscopic alpha measurement system based on the Tensioned Metastable Fluid Detector technology to provide a potential solution for performing rapid gross alpha measurements on these high gamma/beta sample matrices. Measurements using the Indirect Drive Acoustically Tensioned Metastable Fluid Detectors developed as part of this collaboration were performed with an alpha emitting radionuclide. Successful determination of gross alpha activity was observed, indicating a potential pathway for rapid gross alpha measurements in remote-handled shielded cells or in process situations requiring online alpha monitoring. Measurements using this system have been conducted on high beta activity solutions, demonstrating the beta blind capability of this system. Measurements are currently underway to test the system’s capability to measure gross alpha activity on Savannah River Site high level waste high Cs-137 samples that have been measured by the SRNL radiochemistry team. This work was supported by the DOE EM Technology Development program.

DiPrete, David [Savannah River National Laboratory↗

2 νββ spectrum in chiral effective field theory

We investigate two-neutrino double beta decay (2νββ) in chiral effective field theory. We find contributions from weak magnetism and double-weak pion-exchange at next-to-leading-order in the chiral power counting. We discuss the impact of the chiral corrections on the electron spectra and find that they should be included in analyses of 2νββ decay that aim to uncover new physics signatures in the electron spectrum. We illustrate this point by revisiting the effect of sterile neutrinos and non-standard charged interactions. We also find that the pion-exchange contributions involve nuclear matrix elements that are related to those appearing in neutrinoless double beta decay (0νββ). We investigate whether the 0νββ nuclear matrix elements can be obtained from detailed measurements of the energy spectrum of the outgoing electrons in 2νββ transitions.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Evidence for a cytokine-sensitive network of iron-associated genes that protects pancreatic islets against ferroptosis

Background/Objectives: The micronutrient iron is closely connected to inflammation and is among the complex factors contributing to beta-cell failure in diabetes. High levels of dietary iron increase the risk of developing type 2 diabetes, and excessive iron uptake by beta-cells can cause oxidative stress and inhibit function. Elevated levels of proinflammatory cytokines in obese individuals, such as interleukin (IL)-1beta and IL-6, increase the risk of developing type 2 diabetes, and there is evidence that these low levels of circulating cytokines can lead to islet dysfunction. Methods: In this study, gene microarray and other data were analyzed for expression differences in islets treated for 48 h with 10 pg/mL IL-1beta + 20 pg/mL IL-6 as a model of low-grade inflammation versus untreated. Results: Three iron-associated genes were among the most cytokine-sensitive in the mouse genome: Hamp, Steap4, and Lcn2. These proteins are all involved with increasing/retaining cellular iron. We hypothesized that increased cellular iron would lead to increased susceptibility to ferroptosis. Surprisingly, 24 h pre-exposure to low-grade inflammation, which upregulates this iron-gene network, prevented subsequent erastin-induced ferroptosis. We also found that Steap4 overexpression reduced islet dysfunction caused by high-dose proinflammatory cytokines (10× low-dose), suggesting an overall protective effect. Steap4 overexpression also upregulated Hamp and Lcn2, suggesting Steap4 regulates these cytokine-sensitive iron genes.; in contrast, ferritin and ferroportin gene expression, which are not sensitive to cytokines, were unchanged. Conclusions: These data suggest an inflammation-induced network of genes involved in cellular iron uptake and retention plays a protective role in islets against oxidative stress and ferroptosis.

IL-1β↗