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Production of Xenon-135 from isotopically enriched Xenon-134 and Xenon-136 Targets

Atmospheric radioxenon analyses conducted under the Comprehensive Test Ban Treaty Organization (CTBTO) necessitates the collection and analysis of air samples to quantify 135Xe, an indicator for nuclear explosions and reactor operations. Analytical instrument calibration for these analyses requires high quality, monoisotopic reference standards that are typically short lived, and therefore must be produced and shipped promptly to monitoring stations worldwide. This work describes the preparation of 135Xe by neutron capture (n, ?) on monoisotopic 134Xe, neutron irradiation (n,2n) on monoisotopic 136Xe, and high energy photon irradiation (?, n) on monoisotopic 136Xe. The targets are prepared by electromagnetic isotope separation of natural xenon. Results from each process are compared for 135Xe yield and purity.

07 ISOTOPE AND RADIATION SOURCES↗

Angular Correlations of Gamma Rays from Fission Product Solution

Fission products from photon-induced fission are routinely used at Idaho National Laboratory as part of nuclear forensics activities. Typically, the focus is on fission products with relatively large fission yields (Ba-140, Mo-99, etc.). The nuclear data associated with the well-known isotopes have small uncertainties, and many have well-known angular correlations between emitted gamma-rays, if applicable. However, for isotopes with smaller fission yields or less intense gamma-ray emission intensities, the nuclear decay schemes and gamma-ray emission intensities may be less well-known. The Germanium Rotational Measurements for Angular Correlation (GeRMAC) system was designed to use two high-purity germanium (HPGe) detectors in a coincidence counting set-up but allows one of the HPGe detectors to rotate at a constant distance from a radioactive source, changing the relative angle between the two HPGe detectors. Angular correlations can then be determined from the relative photopeak areas between two gamma-rays emitted as part of the same nuclear decay. By recording the HPGe spectra in list mode, the angular correlations of gamma-rays emitted from complex sources, consisting of multiple isotopes, can be measured simultaneously and the individual isotope emissions can be isolated. Using the GeRMAC system, a multi-isotope fission product source, produced with photon-induced fission of U-238, was measured using a single rotational arc (180 degrees) to obtain the angular correlation between gamma-rays emitted by the large number of fission products contained in the solution with an angular accuracy of 1 degree. In particular, La-140 (38 gamma rays) and Nd-147 (26 gamma rays) are of interest to the nuclear forensics community.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

Time projection chamber for GADGET II

The established Gaseous Detector with Germanium Tagging (GADGET) detection system is used to measure weak, low-energy 𝛽-delayed proton decays. It consists of the Gaseous Proton Detector equipped with a MICROMEGAS (MM) readout to detect protons and other charged particles calorimetrically, surrounded by the Segmented Germanium Array (SeGA) for high-resolution detection of prompt 𝛾 rays. To upgrade GADGET's Proton Detector to operate as a compact time projection chamber (TPC) for the detection, three-dimensional imaging and identification of low-energy 𝛽-delayed single- and multiparticle emissions mainly of interest to astrophysical studies. A new high granularity MM board with 1024 pads has been designed, fabricated, installed, and tested. A high-density data acquisition system based on generic electronics for TPCs (GET) has been installed and optimized to record and process the gas avalanche signals collected on the readout pads. The TPC's performance has been tested using a 220 Rn 𝛼-particle source and cosmic-ray muons. In addition, decay events in the TPC have been simulated by adapting the attpcroot data analysis framework. Furthermore, a novel application of two-dimensional convolutional neural networks for GADGET II event classification is introduced. The optimization of data throughput is also addressed. The GADGET II TPC is capable of detecting and identifying 𝛼 particles as well as measuring their track direction, range, and energy. The extracted energy resolution of the GADGET II TPC using P10 gas is about 5.4% at 6.288 MeV ( 220 Rn 𝛼 events), computed using charge integration. Based on a systematic simulation study, we estimated the detection efficiency of the GADGET II TPC for protons and 𝛼 particles, respectively. It has also been demonstrated that the GADGET II TPC is capable of tracking minimum-ionizing particles (i.e., cosmic-ray muons). From these measurements, the electron drift velocity was measured under typical operating conditions. In addition to being one of the first generation of micropattern gaseous detectors (MPGDs) to utilize a resistive anode applied to low-energy nuclear physics, the GADGET II TPC will also be the first TPC surrounded by a high-efficiency array of high-purity germanium 𝛾-ray detectors. As a result, the TPC of GADGET II has been designed, fabricated, and tested and is ready for operation at the Facility for Rare Isotope Beams for radioactive-beam-line experiments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Determination of γ-ray branching ratios for ⁹⁵Zr and ¹⁴⁷Nd

For many fission products, the γ rays emitted following decay provide an easily-detectable signature that can be used to identify their quantities and distributions in a sample. As a result, γ-ray spectroscopy is often exploited to study fission-product yields (FPYs), provided sufficiently accurate information on the γ-ray branching ratio is available. However, in many cases, the uncertainties in the existing nuclear data are large enough that they compromise the precision achievable for modern experiments and applications. To address this need, we have developed a new experimental method that is well suited to precisely measure the γ-ray branching ratios in the decay of long-lived fission products. The approach involves the production of a radiopure sample by implantation of a mass-separated ion beam from the CAlifornium Rare Isotope Breeder Upgrade (CARIBU) facility on a thin carbon foil. The emitted β -decay radiation is detected with a 4π gas proportional counter and a meticulously efficiency-calibrated high-purity germanium (HPGe) detector. As a first measurement to demonstrate the approach, we studied the γ-ray branching ratios of the strongest transitions following the decay of ⁹⁵Zr and decay-daughter ⁹⁵Nb and determined these branching ratios to fractional precisions of 1%. We then applied this approach to determine the γ-ray branching ratios for the β decay of ¹⁴⁷Nd. The results for the γ-ray branching ratios are presented here and compared to previous results and evaluations.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Characterization of the Multi-Coincident Bismuth Germanate Oxide Spectrometer at the Nuclear Counting Facility

A multi-detector γ-ray spectroscopy system including 3 high-purity germanium (HPGe) detectors has been developed at the Nuclear Counting Facility at Lawrence Livermore National Laboratory. This system operates not only in conventional singles γ-ray detection mode but also incorporates features like coincidence and anti-coincidence techniques. These advanced detection modes can significantly enhance the system’s sensitivity, making it a powerful tool for isotope identification and quantification, especially for complex samples with high background and overlapping peaks. In this re port, we present a comprehensive performance characterization of the Multi-Coincident Bismuth Oxide Spectrometer (MCBOS) using a variety of sample types, including 60 Co, 48 Sc, and mixed fission product samples. Each sample provides unique tests for the MCBOS capabilities. Additionally, a GEANT4 model of the MCBOS has been generated to aid with the characterization of the system.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Isotope harvesting from a NSCL beam blocker: Isolation of 173,174 lu

A decommissioned beam blocker from the National Superconducting Cyclotron Laboratory was processed for recovery of long-lived Lu radioisotopes at Lawrence Livermore National Laboratory. The beam blocker was a W alloy that had built up considerable levels of activation from high energy particle irradiation over the course of 20 years. The isolation of 173,174 Lu from the bulk material required a complex chemical separation scheme due to the large mass and the wide variety of elements present. The final yield of 173,174 Lu was 76.7 ± 4.8% with an extremely high radiopurity and chemical purity. The reduction in W mass from the initial material to the final sample was 8 × 10 10 . In conclusion, the results show great promise for extracting large quantities of Lu radioisotopes from these types of W beam blockers at the Facility for Rare Isotope Beams, which will be irradiated at levels significantly higher than the beam blocker investigated here.

and nuclear chemistry↗

Monte Carlo Analysis of Coolant Stream Impurity Gamma Emissions in Gas-Cooled Fast Reactors

It is well established that a rapid increase in the concentration of fission products in the reactor coolant stream can serve as an early indication of fuel failure. We use Monte Carlo simulations to investigate the feasibility of using several gamma detectors as diagnostic equipment to monitor the presence of major fission product isotopes in high-temperature gas-cooled reactor (HTGR) coolant streams for early detection of fuel failure and therefore the prevention of fuel failure conditions. Herein we model the response of high-purity germanium (HPGe), CdZnTe, NaI(Tl), and LaBr 3 (Ce) detectors of typical commercial sizes to the gamma emissions from nuclides expected to be found within the coolant stream of the Versatile Test Reactor (VTR) under development by the U.S. Department of Energy. The results indicate that for the 233- and 250-keV gamma rays from 133 Xe and 135 Xe, respectively, the 3σ detection criterion is met in under 1 min using a single HPGe detector. Changes in other spectral lines associated with Xe nuclides are detected within 1 h regardless of the choice of detector.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Comparison of measurement techniques and sorption of radium-226 in low and high salinity aqueous samples

Human activities have the potential to redistribute radium (Ra) in the marine environment in a manner that may necessitate monitoring or management of subsequent human or environmental exposures. There is therefore a need to identify accurate and accessible techniques for Ra measurement in high salinity samples and to describe the distribution of Ra in estuarine and marine environments, but most efforts in these areas have focused on low salinity matrices. In addition, rapid and reliable measurements are crucial for time-sensitive samples such as short-lived isotopes or emergency situations. The objective of this study is to describe the limits of detection, cost, and relative ease for measurement of Ra in both low and high salinity aqueous samples via three analytical methods: liquid scintillation counting (LSC), high purity germanium (HPGe) gamma spectrometry, and inductively coupled plasma mass spectrometry (ICP-MS). To contextualize these measurements for real-world scenarios, the partitioning of 226 Ra to substrates relevant to the marine environment was also characterized. Although HPGe detection with solid phase extraction had the lowest limit of detection for low salinity samples (0.27 Bq L −1 ), poor 226 Ra recovery for high salinity samples and high materials costs make this method prohibitive for many users. Limits of detection for high salinity samples were lower for LSC (1.28 Bq L −1 ) than for ICP-MS without dilution (11.4 Bq L −1 ), but significant and unexpected degradation of the high salinity LSC standards was observed after six months. Furthermore, our preferred measurement method for high salinity Ra samples is ICP-MS with sample dilution as necessary to reduce matrix effects.

07 ISOTOPE AND RADIATION SOURCES↗

Hexagonal boron nitride: Epitaxial growth and device applications

As a newest family member of the III-nitrides, BN is considered amongst the remaining frontiers in wide energy bandgap semiconductors with potentials for technologically significant applications in deep UV (DUV) optoelectronics, solid-state neutron detectors, electron emitters, single photon emitters, switching/memory devices, and super-capacitors. It was shown that it is possible to produce h-BN epilayers with high hexagonal phase purity, UV transparency, and film stoichiometry by employing nitrogen-rich growth conditions. The quasi-2D nature of h-BN supports unusually strong optical transitions near the band edge and a large exciton binding energy on the order of 0.7 eV. Since the isotope of B-10 has a large capture cross-section for thermal neutrons, h-BN is an ideal material for the fabrication of solid-state neutron detectors for special nuclear materials detection, well and geothermal logging, and medical imaging applications. Freestanding B-10 enriched h-BN (h- 10 BN) epilayers with varying thicknesses up to 200 μm have been successfully synthesized by metal organic chemical vapor deposition (MOCVD) as of this writing. By utilizing the conductivity anisotropy nature of h-BN, 1 cm 2 lateral detectors fabricated from 100 μm thick h-10BN epilayers have demonstrated a detection efficiency of 59% for thermal neutrons, which is the highest on record among all solid-state neutron detectors as of today. It was noted that high growth temperatures, long growth times and the use of sapphire substrate tend to incorporate oxygen related impurities into h- 10 BN epilayers, which strongly impacted the carrier mobility-lifetime (μτ) products and charge collection efficiencies of h- 10 BN neutron detectors. As the h-BN material technology further develops, improved carrier mobilities and μτ products will allow the fabrication of h-BN devices with enhanced performance.

42 ENGINEERING↗

Contributions to the optical linewidth of shallow donor-bound excitonic transition in ZnO

Neutral shallow donors in zinc oxide (ZnO) are spin qubits with optical access via the donor-bound exciton. This spin–photon interface enables applications in quantum networking, memories, and transduction. Essential optical parameters which impact the spin–photon interface include radiative lifetime, optical inhomogeneous and homogeneous linewidth, and optical depth. We study the donor-bound exciton optical linewidth properties of Al, Ga, and In donors in single-crystal ZnO. The ensemble photoluminescence linewidth ranges from 4 to 11 GHz, less than two orders of magnitude larger than the expected lifetime-limited linewidth. The ensemble linewidth remains narrow in absorption through samples with an estimated optical depth up to several hundred. The primary thermal relaxation mechanism is identified and found to have a negligible contribution to the total linewidth at 2 K. We find that inhomogeneous broadening due to the disordered isotopic environment in natural ZnO is significant, contributing 2 GHz. Two-laser spectral hole burning measurements indicate that the dominant mechanism, however, is homogeneous. Despite this broadening, the high homogeneity, large optical depth, and potential for isotope purification indicate that the optical properties of the ZnO donor-bound exciton are promising for a wide range of quantum technologies, and motivate a need to improve the isotope and chemical purity of ZnO for quantum technologies.

Niaouris, Vasileios (ORCID:000000015313748X)↗

Imaging and dosimetric characteristics of 67 Cu

In recent years the use of beta-emitting radiopharmaceuticals for cancer therapy has expanded rapidly following development of therapeutics for neuroendocrine tumors, prostate cancer, and other oncologic malignancies. One emerging beta-emitting radioisotope of interest for therapy is 67 Cu (t 1/2 : 2.6 d) due to its chemical equivalency with the widely-established positron-emitting isotope 64 Cu (t 1/2 : 12.7 h). Here we evaluate both the imaging and dosimetric characteristics of 67 Cu, as well as producing the first report of SPECT/CT imaging using 67 Cu. To this end, 67 Cu was produced by photon-induced reactions on isotopically-enriched 68 Zn at the Low-Energy Accelerator Facility (LEAF) of Argonne National Laboratory, followed by bulk separation of metallic 68 Zn by sublimation and radiochemical purification by column chromatography. Gamma spectrometry was performed by efficiency-calibrated high-purity germanium (HPGe) analysis to verify absolute activity calibration and establish radionuclidic purity. Absolute activity measurements corroborated manufacturer-recommended dose-calibrator settings and no radionuclidic impurities were observed. Using the Clinical Trials Network anthropomorphic chest phantom, SPECT/CT images were acquired. Medium Energy (ME) SPECT collimation was found to provide the best image quality from the primary 185 keV gamma emission of 67 Cu. Reconstructed images of 67 Cu were similar in quality to images acquired using 177 Lu. Recovery coefficients were calculated and compared against quantitative images of 99m Tc, 177 Lu, and 64 Cu within the same anthropomorphic chest phantom. Production and clinical imaging of 67 Cu appears feasible, and future studies investigating the therapeutic efficacy of 67 Cu-based radiopharmaceuticals are warranted.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

Development of an In Situ Fission Gas Release Instrument for Fuel Sample Irradiations in the High Flux Isotope Reactor

Experimental measurement of gaseous fission product release with respect to temperature and burnup is a critical aspect of understanding nuclear fuel performance, validating predictive models, and qualifying new fuels. To measure this phenomenon in real-time, Oak Ridge National Laboratory has developed an instrument for measuring in situ fission gas release from small-scale fuel samples irradiated in the High Flux Isotope Reactor (HFIR). The instrument uses a continuous flow of Heover the fuel samples to sweep gaseous fission products from a sealed capsule in the HFIR Be reflector to an instrument station adjacent to the reactor. The instrument station houses two high-purity germanium (HPGe) detectors that measure decay gamma rays from fission products passing through a room temperature dwell chamber placed over the detector crystal. The sealed capsules in the reactor are designed to modulate fuel sample temperatures between 700 and 1,100°C by changing the Ar/He gas mixture surrounding the capsules during irradiation. N-type thermocouples are incorporated into the capsule housing to record real-time fuel temperatures. The capsules are heated primarily by prompt gamma rays emitted from the HFIR core with minimal heat contributions from fission in the fuel samples to minimize temperature gradients in the specimens for separate-effects characterization of the material. This paper describes modeling of time-dependent nuclear heating and fission product formation in fuel samples, thermal characteristics of the in-core capsules, and expected gaseous fission product gamma spectra at the HPGe instrument station.

Mulligan, Padhraic L [ORNL] (ORCID:000000025826540↗

Application of Gaussian Bayes classifier to differentiate chlorine-based chemical agents

The Portable Isotopic Neutron Spectroscopy (PINS) is a commercialized system developed by Idaho National Laboratory (INL) to examine chemical warfare agents (CWA) non-destructively, utilizing Prompt Gamma Neutron Activation Analysis (PGNAA) techniques. The PINS system takes advantage of a high-resolution gamma-ray spectrum from a mechanically-cooled high-purity germanium (HPGe) detector. One of the difficult technical challenges is to discriminate the chlorine-based chemical agents. Especially, CN, CNB, CNS and CG have similar chemical compositions to make it hard to discriminate them with a higher confidence. Current identification algorithms for PINS systems with 252-Cf sources have been improved and updated continuously as more field data became available, and new algorithms was studied to complement the current algorithms by adopting the Gaussian Bayes classifier. These new algorithms were intended to be applied to a subset of chlorine-based chemical agents, and their main goal is discriminate CN, CNB, CNS and CG with their ratios of the chlorine neutron inelastic 1763keV peak to the chlorine thermal neutron capture 1959keV peak, which is referred to as the “Cl i/c” or “clic” ratio in this study. The Cl i/c ratios were assumed to follow Gaussian distributions with the means and the standard deviations unique to their corresponding chemical agents. The prior probabilities of these four chemical agents were optimized with a collection of field data to achieve the best performance in terms of precision or positive predictive value (PPV). Finally, their posterior probabilities as functions of the Cl i/c ratio were implemented in the current version of PINS analysis software in order to be tested with more field data.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Classification of Dissolution Events Using Fusion of Effluents Measurements and Classifiers

Classifiers for dissolution events at a radiochemical processing facility are studied using gamma spectra measurements of effluents collected by a high purity germanium detector located at its off-gas stack. Data sets collected at the Oak Ridge National Laboratory’s Radiochemical Engineering Development Center under a Pu dissolution campaign spanning a three months period are utilized. Features corresponding to the activity levels of 15 radionuclides, including isotopes of iodine, krypton, and xenon, that are indicated by the target decay chains, are computed from the spectra at 1 hour intervals. A conceptualization diagram is developed to reflect the steps from the source to measurement to feature computation that depend on fission products indicated by decay chains, chemical processing, and effluents transport to the off-gas stack. A diverse set of eight classifiers based on different design principles are trained using the ground truth data for this campaign, and the outputs of top three classifiers, namely, classification trees, Ensemble of Trees (EOT), and k-nearest neighbor, are combined using EOT classifier-fuser. Our results show that for 5-fold cross validation, features associated with isotopes of xenon provide the lowest classification error among the different elements across the classifiers; the classification error is furthered improved when all 15 isotope features are used by each classifier, and it is again improved by the fusion of three classifiers. Further reduction in classification error is achieved by using a measurement window of 1-2 days which is identified based on half-life time estimates of the isotopes; it is long enough for the stabilization of feature estimates while being short enough not to be affected by the follow on dissolution events. As a net result of feature and classifier fusion, combined with the incorporation of decay chain and isotope half-life information, this approach achieves 98% detection rate while maintaining a false alarm rate under 2% for this data set.

Rao, Nageswara↗

AFRRI TRIGA Reactor Neutron and Gamma Dose Characterization Preliminary Results

Integral Experiment Request (IER) 484 is part of a series of dose characterization and nuclear accident dosimeter (NAD) exercises performed under the Department of Energy (DOE) Nuclear Criticality Safety Program (NCSP). The Armed Forces Radiobilogy Research Institute (AFRRI) 1.1 MW Training, Research, Isotopes, General Atomics (TRIGA) Mark-F reactor is the third facility to undergo a dose study to establish reference dose values. A preliminary measurement was performed earlier this year, where a variety of foils were irradiated and activation gamma rays were measured using a high-purity germanium (HPGe) detector. The data was taken and analyzed to calculate the neutron spectrum in the irradiation facility. This paper will present preliminary results of the neutron dose measured. The characterization of the AFRRI dose field is planned in August.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Dense autoencoders, clustering techniques, and semi-supervised learning for HPGe $γ$-spectra

Classifying high-resolution gamma spectra by their isotopic content is an essential task in nuclear forensics and other applications. Traditional analysis methods are often time-intensive, but machine learning (ML) may help analysts quickly process many spectra. Such methods tend to rely on abundant, well-labeled data for training. Historical gamma data exists in various fields but is not uniformly useful for supervised ML due to inconsistent labeling. Here, to address some of these challenges, we present a method to classify and organize unlabeled data from high-purity germanium detectors using an autoencoding neural network (autoencoder). We trained dense autoencoders to compress gamma data into latent representations that enable efficient data characterization. By clustering the encoded spectra or lower-dimensional mappings of them, we identified and removed portions of over-abundant data categories, resulting in a more balanced dataset and improved autoencoder performance. This encoding and clustering pipeline also enabled the organization of spectra into self-consistent categories. Finally, we found that encoded representations showed potential as inputs for semi-supervised learning of nuclide identification (NID) labels, achieving an average F1 score of 0.85 ± 0.03 when mapping encodings to a set of 65 isotope labels.

Autoencoders↗

Simultaneous Separation of Protactinium-230 and Uranium-230 Isotopes from a Proton-Irradiated Thorium Matrix

The use of radioisotopes in cancer therapy is becoming increasingly important. As a potential candidate for targeted alpha therapy, 230 U (t 1/2 = 20.8 d), the decay daughter of 230 Pa (t 1/2 = 17.4 d) is currently being investigated for cancer treatment. For radioisotopes to be used in biomedicine, they must be radiochemically pure and free from carrier interference. This can be challenging given their short half-life. Thus, in this study, radiological separation methods for harvesting isotopes for use in biomedicine must be simple, fast, and capable of obtaining the required purity levels. Herein, we demonstrate a new rapid method for the separation of 230 U and 230 Pa from a proton-irradiated 232 Th metal target and from coproduced fission products with high recovery and purity. A dual-column approach was used, in which the first column was an anion exchange (AX) column and the second column was a DGA column. The MP-1 AX resin was used for the primary separation of the three major components (U, Pa, and Th, as well as fission products), and the DGA column was used for further purification of the separated 230 U. The method is simple and allows for straightforward separation of U, Pa, Th, and fission products; also, the entire process from target dissolution to shipment of 230 U could be completed in 3 days with an overall 230 U recovery yield of 96 ± 3%. Additionally, separated 230 Pa fractions can be used to harvest ingrown 230 U after initial separation.

DGA resin↗

The LLNL rabbit: determination of trace element levels in polyethylene

Rabbit facilities are systems that pneumatically transport a sample carrier (known as a rabbit) to and from a radiation source. However, trace impurities in the polyethylene (PE) rabbit may interfere with measurements of short-lived isotopes. Activated impurities with short half-lives as 28 Al interfere with the fission product γ-ray, therefore the rabbit cannot be measured immediately. Neutron activation analysis was performed on various PE samples obtained from different manufacturers and the highest quality PE was used to fabricate a high-purity PE rabbit. Here, the impurities identified in the PE study were 27 Al, 48 Ca, 37 Cl, 50 Cr, 65 Cu, 127 I, 26 Mg, 55 Mn, and 30 Si.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗