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Multi-Sensor Data Acquisition System for Process Monitoring

Idaho National Laboratory is building a new nuclear fuel cycle test bed. This fuel cycle test bed named “Beartooth” will give researchers the opportunity to study the nuclear fuel cycle process. The process operations include the use of centrifugal contactors and process flow for the purification of special nuclear material recovery in used fuel. This new research facility has the need to use non-traditional measurement sensors to determine the state-of-health of the solvent extraction process. These non-traditional sensors can also enhance nuclear nonproliferation supervision and other activities. The non-traditional sensors include accelerometers, acoustic, current, flow, colorimetric, temperature, pH and conductivity. The challenge behind deploying all these sensors, is the need for fast and reliable data collection. The data acquisition system (DAQ) needs to be capable of recording up to 12 accelerometers and/or acoustic microphones simultaneously at rates up to 12.8 kSamples/second/channel. This requires the need for a strong architecture and data collection solution. This summary identifies the system architecture, DAQ, and sensors needed to support non-traditional measurements in a solvent extraction process.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Use of Machine Learning for Signature Development in a Multi-Sensor Environment for Safeguard Applications of Solvent Extraction Processes

Idaho National Laboratory is constructing the Special Nuclear Material test bed (Beartooth) for research and development pertaining to nuclear fuel processing operations using centrifugal contactors. Beartooth will enable give researchers the opportunity to study the dissolution, separation, and conversion of special nuclear materials (e.g., plutonium, enriched uranium, and thorium). As a lead-in to Beartooth, this project constructed a test bed to study the process and equipment behavior with real time series data collection using a variety of non-traditional sensors, in order to identify process failures and label them as either accidental or purposeful, thus enhancing nuclear nonproliferation stewardship. The measurement sources in this test bed include vibration, acoustic, current, flow, colorimetric, and thermal data. These measurements vary in terms of magnitude, frequency, and location. This information will be combined and used within data-driven machine-learning methods to detect operation condition changes that are either intentional (i.e., changes in operating set points) or malicious (i.e., flow diversion) in nature. This presentation covers the data processing and signature development activities necessary for utilizing this heterogeneous dataset to classify process anomalies.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Intentional Uranium Tagging for Material Provenance and Pathway Forensics (LA19-Intentional-Forensics-NDD3Bb): Final Project Report

This report summarizes the outcomes of a 3-year NA-22 exploratory project to research the feasibility of tagging uranium materials, especially nuclear fuels, for nuclear nonproliferation purposes. The experimental focus was on metallic uranium forms under prospective surface and bulk tagging manufacturing and detection scenarios. This study showed that a large number of tags (drawn from an even larger menu of options) could be successfully imparted and detected in both as-built and degraded conditions. These results pave the way for additional R&D studies of surface and bulk tagging of metallic forms of uranium.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Workshop on Radiographic Imaging and Applications Research and Development Recommendations for Field Radiography

The Workshop on Radiographic Imaging and Applications (WORIA) brought together subject matter experts from industry, academia, US and UK government agencies, and the national laboratories to provide a forum to liaise and share information between technology developers in government and industry, end users, and mission stakeholder to produce an “expert consensus view” regarding future research directions toward a comprehensive radiography/penetrating imaging portfolio in the Defense Nuclear Nonproliferation Research and Development Near Field Detection Portfolio. The inaugural WORIA was held at the Spallation Neutron Source at Oak Ridge National Laboratory on February 7–9, 2023. The inaugural WORIA meeting focused on field radiography applications, or situations in which a portable imaging system must be brought to an item of interest (rather than the item brought to an imaging facility). This report documents consensus views derived from the meeting and provides research and development recommendations for federal program managers.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Empirical Bounding Analysis and User Recommendations for a Neutron Multiplicity Detector

Neutron multiplicity detectors are useful for a variety of applications including nuclear emergency response, nuclear nonproliferation, safeguards, and criticality safety. When measuring black-box problems (i.e., when the system being measured is completely unknown) with systems that have relatively low detection efficiency, expert analysis is frequently required to determine appropriate bounds for system parameters such as neutron multiplication and neutron leakage. This is because the detection efficiency can vary wildly, which also means that the resulting system parameters can have large variations. This work applies an empirical approach to provide bounds on system parameters (such as system multiplication, neutron leakage, and detector efficiency). The results of this bounding analysis are then used as inputs to provide recommendations to users regarding criticality safety. In addition to describing the method used, this work provides sample results from a measurement campaign performed at the National Criticality Experiments Research Center (NCERC).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Realistic application of short-lived fission product delayed neutron, gamma-ray analysis for simultaneous nondestructive trace quantification of U, Pu mixtures on cellulose swipes

Detection and characterization of fissile traces are of interest to the international nuclear nonproliferation community, including the International Atomic Energy Agency. Pre-inspection check samples are analyzed by neutron activation analysis at the High Flux Isotope Reactor operated by the Oak Ridge National Laboratory under the umbrella of the IAEA Network of Analytical Laboratories. The simultaneous quantification of U and Pu mixtures was accomplished using the combined delayed neutron (DN) delayed gamma-ray (DG) method to analyze cellulose swipes with actinide loading <1ng in a blind field trial. The total fissile quantity was measured by the DN counts and the relative proportions of U, Pu were determined by calibration of the 104 Tc / 141 Ba fission product count ratio using known mixtures. The DNDG method demonstrated high accuracy in flagging the presence of 239 Pu in uranium down to <100 pg mass loading. In conclusion, peak significance tests helped to control false positive Pu flagging and simultaneous quantification of U and Pu loading was accomplished on samples that passed the significance tests.

36 MATERIALS SCIENCE↗

Design and Characterization of an Optically Segmented Single Volume Scatter Camera Module

Here, the optically segmented single volume scatter camera (OS-SVSC) aims to image neutron sources for nuclear nonproliferation applications using the kinematic reconstruction of elastic double-scatter events. We report on the design, construction, and calibration of one module of a new prototype. The module includes 16 EJ-204 organic plastic scintillating bars individually wrapped in Teflon tape, each measuring 0.5cx0.5cmx20cm . The scintillator array is coupled to two custom silicon photomultiplier (SiPM) boards consisting of a 2x8 array of SensL J-Series-60035 SiPMs, which are read out by a custom 16 channel DRS4 based digitizer board. The electrical crosstalk between SiPMs within the electronics chain is measured as 0.76%±0.11% among all 16 channels. We report the detector response of one module including interaction position, time, and energy, using two different optical coupling materials: EJ-560 silicone rubber optical coupling pads and EJ-550 optical coupling grease. We present results in terms of the overall mean and standard deviation of the z -position reconstruction and interaction time resolutions for all 16 bars in the module. We observed the 1σz -position resolution for gamma interactions in the 0.3–0.4 MeVee range to be 2.24 cm ± 1.10 cm and 1.45 cm ± 0.19 cm for silicone optical coupling pad and optical grease, respectively. The observed 1σ interaction time resolution is 265 ps ± 29 ps and 235 ps ± 10 ps for silicone optical coupling pad and optical grease, respectively.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Impact of light output on the timing resolution of organic glass scintillator bars in a dual-ended readout configuration

The effectiveness of detector system modeling and validation depends on the quality of characterization performed on the system. For nuclear nonproliferation applications, which require detectors to address complex and variable field conditions, access to accurate system models is essential. This study presents the timing characterization of organic glass scintillator bars used in an imaging system developed at the University of Michigan. 137 Cs and 60 Co gamma-ray sources were used to determine the coincidence time resolution as a function of measured light output for two Compton scatter events between two organic glass scintillator bars. Timing resolution for two events, each with light output ranging from 100 to 1100 keVee were characterized. The resulting data were fit to a parametric function that was validated to agree with experimental results within ±25 ps. Simulations were performed to establish appropriate calibration points for each organic scintillator, thereby ensuring accurate calibration of light output values during analysis. This work successfully characterized the light output dependence of the coincidence timing resolution of a pair of organic glass detectors for use in an imaging system. Depending on the amount of scintillation light output from the events, the full width at half maximum of the measured coincidence time resolution ranged from 653.2 ± 16.1 ps for low light yields, 100 keVee, to 121.0 ± 8.4 ps for higher yields at 1100 keVee. The insights obtained from the timing resolution behavior will allow for accurate simulation capabilities in future security and verification efforts using scatter-based imaging systems.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

High Flux Isotope Reactor Low-Enriched Uranium Low Density Silicide Fuel Design Parameters

High Flux Isotope Reactor (HFIR) highly enriched uranium (HEU) to low-enriched uranium (LEU) conversion activities are ongoing as part of the Department of Energy (DOE) National Nuclear Security Administration (NNSA)’s nuclear nonproliferation mission. Design activities studying the conversion of HFIR from HEU to LEU fuel explored different fuel design features and shapes with a low density uranium-silicide dispersion (U 3 Si 2 -Al) fuel, which has a uranium density of 4.8 gU/cm 3 . The goal of these studies is to generate several HFIR LEU fuel designs of varying fuel fabrication complexity that meet the current HEU performance metrics and safety requirements. The documented designs will serve as references for fuel fabrication and qualification activities. Recent advancements in modeling and simulation tools enable quick prototyping of fuel designs. Shift, a Monte Carlo neutron transport and depletion tool optimized for high-performance computing (HPC) architectures, is used for efficient fuel cycle and performance metrics calculations. The HFIR Steady State Heat Transfer Code (HSSHTC) is used to vet the thermal safety margin. Also, a new automation tool that connects all fuel design analysis steps, named Python HFIR Analysis and Measurement Engine (PHAME), has been developed to expedite the design study in an efficient and reproducible manner. Leveraging these tools, several candidate fuel designs were selected for varying fabrication complexity. This report provides design feature details for four selected HFIR LEU low density U 3 Si 2 -Al fuel designs and their corresponding performance and safety metrics. Nominal, best-estimate design parameters and irradiation conditions, including fission rate densities, power densities, heat fluxes, and cumulative fission densities are provided for candidate fuel designs relevant to framing irradiation experiments to support fuel qualification efforts. Simulations show that the low density U 3 Si 2 -Al, with design features to enhance safety, can meet HEU core performance metrics and safety requirements if the reactor power is increased from 85 MW (HEU) to 95 MW (LEU) and if the active fuel length is increased from 50.80 cm (HEU) to 55.88 cm (LEU).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

High Flux Isotope Reactor Low Enriched Uranium U-10Mo Fuel Design Parameters

Activities to convert the HFIR from HEU to LEU are ongoing as part of the US Department of Energy (DOE) National Nuclear Security Administration (NNSA) nuclear nonproliferation mission. Design activities to study the conversion of HFIR from HEU to LEU fuel explored different fuel design features and shapes with a uranium-molybdenum (U-10Mo) monolithic alloy fuel. This high-density alloy contains 90 wt % uranium and 10 wt % molybdenum and has a uranium density of 15.318gU/cm 3 . The goal of these studies is to generate several candidate HFIR LEU fuel designs of varying fuel fabrication complexity that meet the current HEU performance metrics and safety requirements. Recent advancements in modeling and simulation tools and design methods enabled a thorough analysis of the available design space with U-10Mo fuel. A surrogate model used this analysis as training data to quickly determine the performance of a design given specific design parameters. An optimization module used this surrogate model to quickly search this multidimensional search space given specific desired performance characteristics. This approach was made possible by the large available design space with U-10Mo fuel. Shift, a Monte Carlo tool optimized for high-performance computing (HPC) architectures, was used for faster calculation and better data management for reactor physics simulations. Once most of these design studies were complete, a new suite called the Python HFIR Analysis and Measurement Engine (PHAME) was developed to connect all fuel design analysis steps, making design studies more efficient and reproducible. The post-processing capabilities of these new tools are leveraged for the information provided herein. Leveraging these tools, several candidate fuel designs were selected with varying levels of feature complexity and reactor performance. This report provides design feature details for four selected HFIR LEU U-10Mo fuel designs and their corresponding performance and safety metrics. Nominal best-estimate design parameters and irradiation conditions, including fission rate densities, power densities, heat fluxes, and cumulative fission densities, are provided. Simulations show that the high uranium density of U-10Mo fuel provides a large potential design space that enables various LEU designs to meet HEU core performance metrics and safety requirements with a power increase from 85 MW (HEU) to 95 MW or 100 MW (LEU).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Angular-spectral filtering of recoil protons for optimization of fast neutron imaging employing proton converters

Fast neutron imaging is an important capability for diverse applications such as inertial confinement fusion diagnostics, cargo security, nuclear nonproliferation and arms control, and industrial inspection. Traditional phosphor image plates can be enhanced for fast neutron imaging using hydrogenous plastic converters which allow fast neutrons to scatter off hydrogen nuclei to produce energetic protons that can be recorded by the image plate. However, protons emitted by image plates are not constrained in their emission angle, which contributes to the blur of the resulting image. Here, we investigate two methods that can alter the spatial extent of converted protons that deposit energy in the image plate: reducing the converter thickness, and introducing a proton filter between the plastic converter and image plate to reduce the contribution of lower-energy, off-axis protons to the image. Here we determine the optimal plastic converter thickness for maximizing the signal intensity to be 2–3 mm through Monte Carlo simulations, and we benchmark this result against experimental measurements with a deuterium-tritium (DT) neutron generator. Next, we evaluate the image smearing and signal loss for various converters to show that solely reducing the converter thickness has the expected effect of reducing the blur from proton image smearing of the sharpness of an edge recorded on the image plate at the cost of reducing the signal intensity. The use of a proton filter is shown to achieve a similar improvement of edge sharpness as reducing the converter thickness while also sacrificing the signal intensity. We conclude that the use of proton energy filtering can improve the sharpness of fast neutron images in situations where the converter thickness cannot be reduced below some practical minimum. For more intense neutron sources, the signal intensity is of less concern, and optimizing the resolution of the image plate and therefore of the imaging system could have greater value. In these applications, proton filters may allow for improved fast neutron imaging measurements.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Laser ablation spectrometry for studies of uranium plasmas, reactor monitoring, and spent fuel safety

Nuclear security is one of the defining challenges of our time. Nuclear threats range from deliberate dispersal of radioactive material to contaminate the vital infrastructure to diversion and smuggling of special nuclear material for clandestine nuclear programs and nuclear terrorism, respectively. There is an associated need to develop and sustain the nuclear forensics capabilities, which requires the understanding of complex processes that occur in plasmas of nuclear materials. The area of nuclear safety has seen a resurgence of public interest, and there is a concomitant need to safely store used nuclear fuel and detect structural material failure in nuclear power systems, especially in innovative reactor designs envisioned for future adoption. Laser-produced plasmas are complicated extreme environments that can generate intense and rich, highly specific signatures of nuclear and radiological materials, which can then be explored in a wide range of applications. They include interdiction and rapid detection of nuclear materials, including their isotopic composition, detection over long distances, laboratory simulation of weapons effects, monitoring the condition of structural materials in dry cask storage containers, and novel instrumentation for nuclear power systems. We present a compilation of recent representative examples of the application of laser spectroscopy, and laser-induced breakdown spectroscopy in particular, to nuclear safety and security problems. A case is made that spectroscopic techniques based on laser-produced plasmas offer complementary, and sometimes unique, capabilities that motivate the continued exploration of their efficient production and understanding of the signatures they produce

(020.3260) Isotope shifts, (140.3440) Laser-induce↗

Enhanced Neutron and γ-Ray Detection via 6 Li Substitution in Undoped and Tl-Doped Zero-Dimensional Perovskite Cs 3 Cu 2 I 5 Scintillators

Radiation detectors are crucial in a wide variety of research and commercial applications, such as oil and gas exploration, medical imaging, nuclear nonproliferation, and homeland security. Neutron and gamma-ray detectors are fundamental components in portal monitors at ports and border crossings, bolstering national security against radiological threats. This study presents a dual-mode scintillator, undoped and Tl-doped 6 Li-Cs 3 Cu 2 I 5 , and demonstrates its potential as a promising material for simultaneous thermal neutron and gamma-ray detection. We explore the Bridgman growth of both undoped and thallium doped Li → Cu and Li → Cs substitutional systems with various Li doping levels and assess their impact on scintillation properties. Under 662 keV gamma-ray excitation, the undoped crystals had light yields up to 35,900 ph/MeV, with energy resolutions down to 4.5%. The Tl-doped crystals performed better than the undoped crystals with light yields peaking at 65,900 ph/MeV and energy resolutions as low as 3.5%. When exposed to a moderated 252 Cf excitation source, our crystals had light yields between 102,900 and 167,200 photons per thermal neutron capture, with a full energy thermal neutron peak reaching 3 MeV in gamma equivalent energy. Pulse shape discrimination studies reveal well-separated gamma and neutron events, resulting in Figure-Of-Merit (FOM) as high as 3.7. Furthermore, these findings highlight the potential of Li-doped Cs 3 Cu 2 I 5 as a viable candidate for next-generation dual-mode scintillators.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

From Fluid Flow to Coupled Processes in Fractured Rock: Recent Advances and New Frontiers

Abstract Quantitative predictions of natural and induced phenomena in fractured rock is one of the great challenges in the Earth and Energy Sciences with far‐reaching economic and environmental impacts. Fractures occupy a very small volume of a subsurface formation but often dominate fluid flow, solute transport and mechanical deformation behavior. They play a central role in CO 2 sequestration, nuclear waste disposal, hydrogen storage, geothermal energy production, nuclear nonproliferation, and hydrocarbon extraction. These applications require predictions of fracture‐dependent quantities of interest such as CO 2 leakage rate, hydrocarbon production, radionuclide plume migration, and seismicity; to be useful, these predictions must account for uncertainty inherent in subsurface systems. Here, we review recent advances in fractured rock research covering field‐ and laboratory‐scale experimentation, numerical simulations, and uncertainty quantification. We discuss how these have greatly improved the fundamental understanding of fractures and one's ability to predict flow and transport in fractured systems. Dedicated field sites provide quantitative measurements of fracture flow that can be used to identify dominant coupled processes and to validate models. Laboratory‐scale experiments fill critical knowledge gaps by providing direct observations and measurements of fracture geometry and flow under controlled conditions that cannot be obtained in the field. Physics‐based simulation of flow and transport provide a bridge in understanding between controlled simple laboratory experiments and the massively complex field‐scale fracture systems. Finally, we review the use of machine learning‐based emulators to rapidly investigate different fracture property scenarios and accelerate physics‐based models by orders of magnitude to enable uncertainty quantification and near real‐time analysis.

58 GEOSCIENCES↗

Remote sensing of Pu in uranyl nitrate crystals using reflectance spectroscopy and chemometrics

Remote quantification of Pu(VI) (0–5 mol%) co-crystallized with U in uranyl nitrate hexahydrate (UNH) crystals was achieved in a glove box using reflectance spectroscopy coupled with chemometric modeling. Reflectance spectra were also acquired for Pu(IV) and Np(VI) (0–5 mol%) crystallized with UNH; revealing spectral features consistent with their solution-phase analogs. Principal component analysis revealed Pu(IV/VI) and Np(VI) concentrations as the primary source of variation in the data, informing the development of a supervised partial least squares regression model for Pu(VI). The resulting calibration demonstrated robust performance, with replicate root mean square errors near 10% and quantifiable limits near 0.2 mol% Pu(VI) relative to U. The Pu(VI) remained stable in the crystalline UNH matrix for at least one week with minimal reduction to Pu(IV). Notably, Pu(VI) and Np(VI) incorporation in UNH quenched U(VI) fluorescence while Pu(IV) did not. This study presents a noninvasive, spectroscopic approach for solid-state Pu quantification, with direct implications for material accountability and nuclear nonproliferation monitoring.

Sadergaski, Luke R. [Oak Ridge National Laboratory↗

Optimization of selenium in CdZnTeSe quaternary compound for radiation detector applications

X- and gamma-ray detectors are increasingly becoming essential tool for science and technology in various fields include homeland security, nonproliferation, nuclear security, medical imaging, astrophysics, and high energy physics. Cd 1-x Zn x Te 1-y Se y (CZTS) is emerging as a next-generation compound semiconductor for such applications. CZTS was found to possesses a very low concentration of Te inclusions and free from sub-grain boundary networks. Being a quaternary compound with varying alloy composition, optimization of the composition was performed to determine the minimum amount of selenium required to produce CZTS with reduced defects. The optimized composition was found to be x=0.10 and y=0.02, i.e., Cd 0.9 Zn0.1Te 0.98 Se 0.02 , for excellent material properties as a radiation detector. The resulting material was free from sub-grain boundary networks and with a highly reduced concentration of Te inclusions. The bulk dark resistivity obtained was in the range of 1-3x1010 ohm-cm with the highest achieved mobility-lifetime product of ~6.6x10-3 cm2/V for the optimized CZTS composition. Impurity analyses were performed by the Glow Discharge Mass Spectroscopy (GDMS) technique, and the results showed relatively high impurity concentrations compared to commercial detector-grade CdZnTe. Thus, CZTS has room for further improvement with additional purification of the starting materials.

36 MATERIALS SCIENCE↗

Anticipating Technical Expertise and Capability Evolution in Research Communities Using Dynamic Graph Transformers

The ability to anticipate global technical expertise and capability evolution trends is essential for national and global security, especially in safety-critical domains such as nuclear nonproliferation (NN) and rapidly emerging fields like artificial intelligence (AI). Here, in this work, we extend traditional statistical relational learning approaches (e.g., link prediction in collaboration networks) and formulate a problem of anticipating technical expertise and capability evolution using dynamic heterogeneous graph representations. We develop novel capabilities to forecast collaboration patterns, authorship behavior, and technical capability evolution at different granularities (e.g., scientist and institution levels) in two distinct research fields. We implement a dynamic graph transformer (DGT) neural architecture, which pushes the state-of-the-art graph neural network models by: 1) forecasting heterogeneous (rather than homogeneous) nodes and edges; and 2) relying on both discrete- and continuous-time inputs. We demonstrate that our DGT models predict collaboration, partnership, and expertise patterns with 0.26, 0.73, and 0.53 mean reciprocal rank values for AI and 0.48, 0.93, and 0.22 for NN domains. DGT model performance exceeds the best-performing static graph baseline models by 30%–80% across AI and NN domains. Our findings demonstrate that DGT models boost inductive task performance when previously unseen nodes appear in the test data for the domains with emerging collaboration patterns (e.g., AI). Specifically, models accurately predict which established scientists will collaborate with early career scientists and vice versa in the AI domain.

97 MATHEMATICS AND COMPUTING↗

Real-Time, Adaptive Radiological Anomaly Detection and Isotope Identification Using Non-Negative Matrix Factorization

Spectroscopic anomaly detection and isotope identification algorithms are integral components in nuclear nonproliferation applications such as search operations. The task is especially challenging in the case of mobile detector systems because the observed gamma-ray background changes more than for a static detector system, and a pretrained background model can easily find itself out of domain. The result is that algorithms may exceed their intended false alarm rate or sacrifice detection sensitivity to maintain the desired false alarm rate. Non-negative matrix factorization (NMF) is a powerful tool for spectral anomaly detection and identification, but, like many similar algorithms that rely on data-driven background models, in its conventional implementation, it is unable to update in real time to account for environmental changes that affect the background spectroscopic signature. Here, we have developed a novel NMF-based algorithm that periodically updates its background model to accommodate changing environmental conditions. The adaptive NMF algorithm involves fewer assumptions about its environment, making it more generalizable than existing NMF-based methods while maintaining or exceeding detection performance on simulated and real-world datasets.

Anomaly detection↗