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54 records · Page 3

Contrastive Machine Learning with Gamma Spectroscopy Data Augmentations for Detecting Shielded Radiological Material Transfers

Data analysis techniques can be powerful tools for rapidly analyzing data and extracting information that can be used in a latent space for categorizing observations between classes of data. Machine learning models that exploit learned data relationships can address a variety of nuclear nonproliferation challenges like the detection and tracking of shielded radiological material transfers. The high resource cost of manually labeling radiation spectra is a hindrance to the rapid analysis of data collected from persistent monitoring and to the adoption of supervised machine learning methods that require large volumes of curated training data. Instead, contrastive self-supervised learning on unlabeled spectra can enhance models that are built on limited labeled radiation datasets. This work demonstrates that contrastive machine learning is an effective technique for leveraging unlabeled data in detecting and characterizing nuclear material transfers demonstrated on radiation measurements collected at an Oak Ridge National Laboratory testbed, where sodium iodide detectors measure gamma radiation emitted by material transfers between the High Flux Isotope Reactor and the Radiochemical Engineering Development Center. Label-invariant data augmentations tailored for gamma radiation detection physics are used on unlabeled spectra to contrastively train an encoder, learning a complex, embedded state space with self-supervision. A linear classifier is then trained on a limited set of labeled data to distinguish transfer spectra between byproducts and tracked nuclear material using representations from the contrastively trained encoder. The optimized hyperparameter model achieves a balanced accuracy score of 80.30%. Any given model—that is, a trained encoder and classifier—shows preferential treatment for specific subclasses of transfer types. Regardless of the classifier complexity, a supervised classifier using contrastively trained representations achieves higher accuracy than using spectra when trained and tested on limited labeled data.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Replacing photomultiplier tubes with silicon photomultipliers for nuclear safeguards applications

Photomultiplier tubes (PMTs) have been used for decades as the default light detection technology for scintillator-based radiation monitors. PMTs come with a handful of disadvantages, however, including large volume usage, fragility, high-voltage requirements, and susceptibility to magnetic fields. Arrays of silicon photomultipliers (SiPMs) are a possible alternative to PMTs providing similar performance while offering improvements in the areas listed. We focus on straightforward “drop-in replacement” evaluations by imposing a single channel output of the SiPM signal and a backend electronics data acquisition and analysis routine identical to that used for PMTs. In the realm of nuclear safeguards, the primary performance metric for gamma spectroscopy is detector resolution, and for neutron detection it is pulse shape discrimination (PSD) to separate neutron and gamma signals. In this work we present the results of replacing a PMT with a 2” x 2” SiPM array mounted, in turn, to the same 2” x 2” cylindrical sodium iodide (NaI) crystal. The ultimate comparison for this gamma spectrometry is confirmation of uranium enrichment standards, ranging from depleted uranium to 93% highly enriched uranium (HEU), by analyzing the resulting spectra with both a simple integral scaling in key energy regions of the spectrum, as well as with the NaIGEM software package. In addition to the gamma spectroscopy work, we will present the latest results on comparing the PSD capabilities of a 4” x 4” SiPM array to a 5” PMT. As with the gamma spectroscopy evaluations, the light detectors are mounted in turn to the same liter-scale organic scintillators. This neutron-focused work includes evaluation of prototype SiPM readout boards with a single output signal summed over 256 individual SiPM pixels, and evident tradeoffs between PSD capability and fast response.

Engineering - Instrumentation related to nuclear s↗

AMS / BARC Joint Survey Addendum Technical Report

This report details the data analysis results from data collected during the September-October 2019 joint survey series between the Department of Energy (DOE) National Nuclear Security Administration (NNSA) Aerial Measuring System (AMS) asset, and the Government of India’s Department of Atomic Energy (DAE) Bhabha Atomic Research Centre (BARC). This joint survey series took place at the Nevada National Security Site (NNSS), areas of public land in Southern Nevada, and at the DOE Office of Legacy Management (LM) Large Area Calibration Pads (LACP) at the Grand Junction Regional Airport in Grand Junction, CO. The data detailed in this report were gathered at the LACP. More details regarding the setup of these surveys and personnel involvement can be found in the AMS / BARC Joint Survey Summary Report. The data from the LACP collected by AMS are consistent with past data collection campaigns at the LACP. The AMS Bell 412 (B412) helicopter, equipped with both the standard AMS thallium-doped sodium iodide (NaI(Tl)) 2"x4"x16" 12-detector system and a subset of the BARC Aerial Gamma Spectroscopy System (AGSS) consisting of two independent 3"x3"cylindrical NaI(Tl) detectors, measured each of the five calibration pads for a minimum of 10 minutes. After the helicopter measurements, a pressurized ion chamber (PIC) was used to directly measure radiation exposure rates on each of the pads for a period 5 minutes. The geophysical calibration procedure published by the International Atomic Energy Agency (IAEA) (Erdi-Krausz et al. 2003) was used to determine the spectral stripping sensitivity matrix for naturally occurring radiological material (NORM). The sensitivity matrix is consistent with the AMS long term average. Additionally, the PIC data was used to calibrate the AMS system for exposure rate. The results of the exposure rate analysis are also consistent with AMS long-term averages.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Quantity of 135I Released from the AGR 5/6/7 Experiment

A series of four Advanced Reactor Technologies (ART) experiments have been conducted in the Advanced Test Reactor (ATR) at Idaho National Laboratory (INL). From 2006 through 2020, these experiments supported the development and qualification of the new U.S. tristructural isotropic (TRISO) particle fuel for Very High Temperature Reactors (VHTR). Each Advanced Gas Reactor (AGR) experiment consisted of multiple fueled capsules, each plumbed for independent temperature control using a mix of helium and neon gases. The gas leaving a capsule was routed to individual Fission Product Monitor (FPM) detectors. For intact fuel particles, the TRISO particle coatings provide a substantial barrier to fission product release. However, particles with failed coatings, whether because of a minute percentage of initially defective particles, those which fail during irradiation, or those designed to fail (DTF) particles, can release fission products to the flowing gas stream. Because reactive fission product elements like iodine and cesium quickly deposit on cooler capsule components and piping structures as the effluent gas leaves the reactor core, only the noble fission gas isotopes of Kr and Xe tend to reach FPM detectors. The FPM system utilizes High Purity Germanium (HPGe) detectors coupled with a thallium activated sodium iodide NaI(Tl) scintillator. The HPGe detector provides individual isotopic information, while the NaI(Tl) scintillator is used as a gross count rate meter. During irradiation, the 135mXe concentration reaching the FPM detectors is from both direct fission and by decay of the accumulated 135I. About 2.5 hours after irradiation (ten 15.3 minute 135mXe half lives) the directly produced 135mXe has decayed and only the longer lived 135I remains as a source. Decay systematics dictate that 135mXe will be in secular equilibrium with its 135I parent, such that its production rate very nearly equals the decay rate of the parent, and its concentration in the flowing gas stream will appear to decay with the parent half life. This equilibrium condition enables the determination of the amount of 135I released from the fuel particles by measurement of the 135mXe at the FPM following reactor shutdown. In this paper, the 135I released will be reported.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High fidelity ground deposition measurement with robots after explosive radiological dispersion

A team of scientists from the Remote Sensing Laboratory at Joint Base Andrews, Maryland, has assembled a remote-controlled robot to field a few sodium iodide scintillators of different size and shape 18″ above ground for measurement of ground deposition of gamma-emitting particles after an explosion of a radiological dispersal device. This system uses a high-precision differential GPS device with submeter accuracy for radiation mapping. The system is most useful in characterizing large-area contamination and detecting gamma radioactivity in invisible, submicron particulate debris deposited on the ground at surface level or embedded in subsurface up to 3″ deep. The system was assembled as part of a larger effort to integrate advanced radiological detection devices into autonomous or remote-controlled robotic systems to eliminate or minimize the need for emergency responders to enter areas that pose significant health and safety risks to humans following a major radiological incident or accident. Research into autonomous algorithms is required to develop automated robotic systems for radiological survey and characterization activities in highly contaminated areas. The scope of this project also includes developing communications pathways and supporting infrastructure capabilities for different types of robotic technologies. The expected result is an advanced autonomous robotic system with integrated radiation detection electronics that allows emergency response personnel to view data remotely and in real time for radiological emergency response and consequence management purposes.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Characterization of Scintillating Crystal for High Energy Radiation Detection and Applications

Cesium Hafnium Chloride (Cs2Hfl6) is a promising metal halide scintillating detector due to its excellent characteristics such as non-hygroscopicity, high light yield without doping. Scintillators plays an important role in nuclear security applications as detectors at border monitoring stations. We grew and characterized CHC crystals to be fabricated for gamma detection. Photoluminescence was performed using the Duetta Fluorescence and Absorbance Spectrometer. The energy response to Cs-137 and Co-60 reference sources was recorded for a representative sodium iodide (NaI) scintillating detector.

Reeder, Angel↗

Spectra-to-exposure conversion using polynomial response models for gamma-ray field characterization

Accurate measurement of exposure rate from gamma-ray spectral data remains a critical challenge during radiological emergency response operations. Conventional methods rely on pre-defined static conversion factors derived from fixed geometries and isotopic compositions, which often fail to capture real-world environmental variability. This study presents a generalized approach as a "next-step" for converting gamma-ray spectral data into exposure rate using polynomial response models. The method introduces a flexible weighting scheme based on the in-situ detector response to distributed sources, enabling a pathway towards improved correspondence between measured spectra and "ground-truth" exposure rates. Experimental data from sodium iodide NaI(Tl) detectors were used to validate the approach as, at least equivalent to the current count-to-exposure method employed in emergency response CONOPS. Results show that the polynomial weighting model is sufficiently equal to the count-to-exposure method and may help improve accuracy given its adaptability to real-world conditions.

61 RADIATION PROTECTION AND DOSIMETRY↗

Low temperature sodium battery comprising an electrochemically active molten inorganic catholyte

A high-performance electrochemically active sodium molten salt catholyte enables a dramatic reduction in molten sodium battery operating temperature from near 300° C. to less than 120° C. As an example, stable electrochemical cycling was demonstrated in a high voltage (3.65 V) sodium battery comprising a sodium iodide-gallium chloride (NaI—GaCl 3 ) molten salt catholyte for over 8 months at 110° C. The combination of high voltage, stable cycling behavior, and practical current densities supported by a molten catholyte enables a new generation of transformative high performance, low temperature molten sodium batteries.

Spoerke, Erik D.↗

Biogeochemistry of the Antrim Shale Natural Gas Reservoir

The Antrim Shale, located in the Michigan Basin, United States (U.S.), is a major U.S. shale play having produced over 2.5 Trillion Cubic Feet (Tcf) of unconventional shale natural gas as of 2010. The shallow nature of this formation sets it apart from other, more characterized unconventional shale gas plays. The depth of gas production of the Antrim ranges from approximately 150 to 600 m and it is typically vertically drilled, contrary to deeper, horizontally drilled shales. A thorough understanding of the biogeochemistry and microbiology of this complex system will be advantageous for improving well performance, produced water management, and potential biocidal treatment as microbial community composition can vary substantially even among closely spaced wells. In this study, we analyzed produced water collected from nine different wells in the Antrim Shale by investigating the geochemical and microbial community composition of the produced water to gain greater insight into the overall biogeochemistry of this unique shale system. The majority of the wells from this study had high total dissolved solids (TDS) primarily composed of chloride and sodium, averaging 86,804 mg/L with a maximum 116,223 mg/L; however, three of the wells sampled along the northern margin of the basin exhibited significantly lower TDS ranging from 4932 to 6496 mg/L. Overall, our microbial community analysis revealed relatively low abundance within our samples and high variability of the microbial community among the sampled wells. The majority of bacterial sequences were identified within Proteobacteria, Firmicutes, and Actinobacteria phyla and metagenomic sequencing revealed the low presence of Methanobacteriaceae within each sample. We also investigated potential microbial community drivers and found that TDS, sodium, chloride, iodide, bromide, ammonium, potassium, and strontium were significantly correlated with the observed microbial community. The varying geochemical conditions between wells demonstrate different subsurface environmental niches, potentially driving the heterogeneous microbial communities we observed from well to well. This analysis suggests an important relationship between both well location and geochemistry and the observed microbial community that can persist in the reservoir. Continued studies of the Antrim Shale will improve our understanding of the complex interdependencies of this ecosystem.

03 NATURAL GAS↗

Extremely Low Energy Nuclear Recoil Calibrations for Dark Matter Direct Detection (Final Technical Report)

This project developed and demonstrated a new calibration approach for low-energy nuclear recoils in solid-state detectors based on neutron capture. Precise calibration in the sub-keV regime is a critical challenge across the HEP portfolio. Existing measurements show deviations and inconsistencies across methods. Neutron capture provides a complementary approach producing discrete recoils via γ cascades.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Large Volume Airborne Contamination Monitoring To Support Nuclear Processes' Deactivation and Decommissioning

Current D and D operations at Hanford have demonstrated a flaw in the current state of the art capability of defining airborne contamination boundaries - Airborne particulate emissions of Pu-239 from CM2H operations on the Hanford Pu Finishing Plant were detected well beyond areas controlled for airborne Pu, putting numerous workers at risk for radiological assimilations - Current air samplers and CAM systems were surveying insufficient volumes of air to accurately predict where respiratory protection was required - Hanford is located in a high radon environment, making air monitoring for alpha emitting actinides challenging in high alpha radon induced backgrounds. - Inexpensive HEPA based home and industrial air purifiers filter significantly higher volumes of air than commercially available continuous-air monitoring (CAM) systems. - Inexpensive models capable of filtered air volumes exceeding 1000 times that of a CAM. - Detector system can be built to detect x-rays generated from actinide decay. - Branching ratios of x-rays are 4 orders of magnitude more intense from Plutonium decay than its gamma emissions. - Detector system can be a low resolution systems, as x-ray region of interest is not terribly congested. - Detection systems evaluated will be designed based on slabs of NaI or pixelated NaI or CsI panels. - Simple graphical user interface software will be developed to operate the detection system. - Concept is to deploy some of these air-purifying systems in nonradiological areas around SRNL to confirm radon can be rejected with confidence. - Generate some filters contaminated with plutonium via electroplated Pu or lab generated simulated particles. - then deploy units in known airborne radiological environments to establish systems ability to accurately measure actinide based hot particles Lab analyses will follow up the system analyses to ensure hot particles were correctly identified. Analysis by Scintillation: - Application of scintillation media to the surface of the filters is being explored. - Evaluating slabs of ZnS(Ag), application of powdered ZnS(Cu) and spray on Perkin Elmer Enhance. - Scintillation events would then be digitized with a digital camera and quantified. - Comparing against sensitivity of a PMT or SiPD readout. - Currently evaluating a Thorlabs 8 Megapixel Monochrome Scientific CCD Camera, hermetically sealed cooled package with a wide angle lens. - Wide angle lens allows complete view of HEPA filter from 7 inches away. - Images taken of glow in the dark paint, as well as plutonium-induced fluorescence. - Plutonium was flamed mounted on a 1 inch diameter stainless steel planchet, covered with a layer of mylar and a section of scintillating ZnS obtained from Eljon. - Currently working on reducing signal-to-noise levels to boost sensitivity. - Dark box to hold contaminated or electroplated source covered filters under fabrication. Analysis by x-ray Spectroscopy: - Branching ratios for x-ray emissions from Plutonium isotopes are orders of magnitude more intense than gamma-ray emissions. - The nuclear databases are incomplete on the branching ratios of some of the isotopes. - Evaluating some custom built SrI2 x-ray spectrometers vs a conventional windowed NaI detector. - SrI2 detectors are carbon-composite-windowed 51 mm x 51 mm. - MCNP calculations to establish self absorbance of filter media on 17 keV x-ray. Radon Rejection: - Activated charcoal pre-filter acts as a Radon trap. - Adding a time lapse feature to camera to aid in radon rejection. SRS Plutonium Fuel Form D and D Operations: Currently deploying air sampler to D and D operation of Pu-238 facility at SRS to generate some field samples to analyze.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Hemicellulose and starch citrate chitosan foam adsorbents for removal of arsenic and other heavy metals from contaminated water

Arsenic and other heavy metal contaminants in water are a significant global health threat. In this study, low-cost, sulfur-free, sustainable, water-insoluble materials with heavy metal remediation properties were produced from renewable resources such as starch, xylan, citric acid, and chitosan. Synthesized starch citrate-chitosan (SCC) foam and xylan citrate-chitosan (XCC) foam were flexible, porous, and elastic. The foams’ arsenic uptake in water was significantly greater than five different commercial metal remediating agents. The mercury and lead uptakes with the synthesized foams were similar to the performance of a commercial sulfur-based product, SorbaTech 450 (ST450). However, the cadmium and selenium uptakes were comparatively lower. The complexation of arsenic with oxygen and nitrogen of the SCC foam was shown with time-of-flight secondary ion mass spectrometry (TOF-SIMS). The XCC foam was also shown to adsorb potassium iodide (KI) at a similar rate to sodium chloride. This may be used to remediate water contaminated with radioactive materials, such as iodine 131.

Materials Science↗

Iodide uptake by forest soils is principally related to the activity of extracellular oxidases

129 I is a nuclear fission decay product of concern because of its long half-life (16 Ma) and propensity to bioaccumulate. Microorganisms impact iodine mobility in soil systems by promoting iodination (covalent binding) of soil organic matter through processes that are not fully understood. Here, we examined iodide uptake by soils collected at two depths (0–10 and 10–20 cm) from 5 deciduous and coniferous forests in Japan and the United States. Autoclaved soils, and soils amended with an enzyme inhibitor (sodium azide) or an antibacterial agent (bronopol), bound significantly less 125 I tracer (93%, 81%, 61% decrease, respectively) than the untreated control soils, confirming a microbial role in soil iodide uptake. Correlation analyses identified the strongest significant correlation between 125 I uptake and three explanatory variables, actinobacteria soil biomass ( p = 6.04E-04, 1.35E-02 for Kendall-Tau and regression analysis, respectively), soil nitrogen content ( p = 4.86E-04, 4.24E-03), and soil oxidase enzyme activity at pH 7.0 using the substrate L-DOPA ( p = 2.83E-03, 4.33E-04) and at pH 5.5 using the ABTS ( p = 5.09E-03, 3.14E-03). Together, the results suggest that extracellular oxidases, primarily of bacterial origin, are the primary catalyst for soil iodination in aerobic, surface soils of deciduous and coniferous forests, and that soil N content may be indicative of the availability of binding sites for reactive iodine species.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dendrite inhibiting electrolytes for metal-based batteries

A metal-based battery includes at least one metal electrode immersed within an electrolyte that includes: (1) an aprotic solvent; (2) a simple halogen containing material; and (3) optionally a metal salt that includes a complex halogen containing anion. The simple halogen containing material may include a metal halide salt that includes a metal cation selected from the group including but not limited to lithium and sodium metal cations. The metal halide salt may also include a halide anion selected from the group consisting of fluoride, chloride, bromide and iodide halide anions. The use of the metal halide salt within the metal-based battery provides enhanced cycling ability within the metal-based battery. Also contemplated are additional simple halogen containing material additives that may enhance cycling performance of a metal-based battery.

Archer, Lynden A.↗

Performance of CsI:Tl Cyrstal with a Spectrum Matching Photomultiplier Tube

This report documents an effort to improve the energy resolution for a thallium doped cesium iodide (CsI:T1) scintillator paired with a spectrum matching photomultiplier tube (PMT). A comparison of the differences in the pulse height spectra from thallium doped (CsI:T1) and sodium doped (CsI:Na) single crystals with PMTs of different spectrum responses was performed. Results show that energy resolution of the detector only improves 0.5% at room temperature when these scintillators are coupled with a spectrum matching PMT. Based on a spectrum matching PMT, the best results for energy resolution are 7.39% and 7.88% for CsI:T1 and CsI:Na scintillators, respectively. The improvement is primarily attributed to the increase of photon statistics from the increase of photons (N) being detected in the spectrum matching PMT. Other factors, such as optical quantum yield and non-proportionality of the CsI:T1 and CsI:Na crystals, that can affect the energy resolution were also studied and reported. The results indicate that although the use of a spectrum matching PMT enhances the photon statistics, it also exacerbates the nonproportionality response. Consequently, a promised improvement on energy resolution due solely to photon statistics was not fully realized.

36 MATERIALS SCIENCE↗

Spectroscopic features of dissolved iodine in pristine and gamma-irradiated nitric acid solutions

While iodine speciation is important for a wide range of nuclear activities, understanding the mechanisms of the transformations of iodine between chemical forms and the sensitivity of these transitions to solution conditions and exposure to radiation remains an active area of research. This work curates spectroscopic data from several experimental techniques and establishes their sensitivity and limitations in detecting changes in iodine speciation in both neutral and acidic regimes. The techniques include Raman spectroscopy, Fourier Transform Infrared (FTIR) spectroscopy, 127 I NMR spectroscopy, and ultraviolet-visible (UV-Vis) spectroscopy. Analysis of these data indicates that these commonly accessible spectroscopies often have dynamic ranges of measurable concentrations that do not always overlap between all techniques. The experimental techniques are disparately sensitive to iodide (I - ), molecular iodine (I 2 ), iodate (IO 3 - ), and periodate (IO 4 - ) species. Raman, FTIR, and NMR spectra were subsequentially analyzed using two-dimensional correlation analyses to generate high-resolution autocorrelation spectra. Here, the use of these spectroscopies is then extended to tracking acidification-induced and gamma irradiation-induced transformations of dissolved sodium iodate in deionized water and concentrated nitric acid. Both dissolution into nitric acid and irradiation with a gamma source are demonstrated to perturb the iodine speciation promoting their assembly into molecular iodine (I 2 ) and/or triiodide (I 3 - ). While I 2 and I 3 - species are undetectable with FTIR spectroscopy and 127 I NMR spectroscopy, the species can be detected with UV-Vis spectroscopy, and in some instances, I 3 - can be detected with Raman spectroscopy in the low wavenumber region. Ultimately, the results of this work provide a path to designing optimal combinations of techniques to detect forms of iodine across a wide range of concentrations and conditions.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗