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Advances in Autoradiography Systems for Nuclear Forensic Analysis

Nuclear forensic analysis techniques work to determine the contents of radiological samples with nondestructive and destructive analysis methods. Autoradiography is a nondestructive analysis method that creates an image of the distribution of radioactivity within the sample. These images allow the location of the radiological content within a sample to be ascertained, which can be used for further analysis. Autoradiography has been used since the discovery of radiation and has been continuously developed to better suit the needs of the medical, nuclear security, nuclear safeguards, and nuclear forensic communities. Recent developments in autoradiography have led to a higher spatial resolution down to a level of tens of microns, real-time capabilities that minimize the risk of overexposure, and the ability to discriminate particles. All of these developments in autoradiography would assist the nuclear forensics community in understanding the placement of radiological content within a sample and in understanding the locations of beta-particle interactions versus those for alpha-particle interactions. This article aims to discuss the history of autoradiography as well as multiple different autoradiographic technologies while focusing on imaging plates, the BeaQuant system, and the ionizing-radiation Quantum Imaging Detector system. This article reviews three autoradiographic techniques and detectors, discusses how they relate to nuclear forensics, and addresses the drawbacks and benefits of each detector.

Autoradiography↗

DRiFT - Release 1.0.0 Organic Scintillators

DRiFT (a Detector Response Function Toolkit) is LANL-developed software that postprocesses output from the extensively validated radiation transport code, MCNP [1], and generates realistic nuclear instrumentation response. DRiFT is designed to be flexible, enabling users to specify detector type and many experimental settings, as well as accommodating the addition of their own desired features. Although DRiFT development has included scintillator [2], gas [3], and semiconductor features [4], the focus of this release is on organic scintillator and associated capabilities. Organic scintillators are widely used in the areas of nuclear safeguards and nuclear non-proliferation efforts [5, 6]. DRiFT has several diagnostic and detector physics features relevant to detailed scintillator simulations including: tracking source particle information, scintillation light production, the effects of PMT quantum efficiency and gain, and digitizer settings. Users can select responses from many scintillator and PMT types supported natively by DRiFT, or add their own by following the instructions in this document. We acknowledge that DRiFT is under active development, bug reports and general questions and comments should be directed to Madison Andrews, madison@lanl.gov. This manual is divided into four parts: I) An overview of DRiFT, including how to obtain and install the executable, II) A description of the detector physics related to scintillators available, III) a description of more general DRiFT features the user may find useful, and IV) a description of the test suite and examples made available with the code release.

61 RADIATION PROTECTION AND DOSIMETRY↗

DRiFT - Release 2.1.0: Organic Scintillators and Gas Detectors

DRiFT (a Detector Response Function Toolkit) is LANL-developed software that post-processes output from the extensively validated radiation transport code, MCNP, and generates realistic nuclear instrumentation response. DRiFT is designed to be flexible, enabling users to specify detector type and many experimental settings, as well as accommodating the addition of their own desired features. The focus of this release is on organic scintillator, gas detector, and associated capabilities, while semiconductor features are still under development. Organic scintillators are widely used in the areas of nuclear safeguards and nuclear non-proliferation efforts. DRiFT has several diagnostic and detector physics features relevant to detailed scintillator simulations including: tracking source particle information, scintillation light production, the effects of PMT quantum efficiency and gain, and digitizer settings. Users can select responses from many scintillator and PMT types supported natively by DRiFT, or add their own by following the instructions in this document. DRiFT also has several diagnostic and detector physics features relevant to neutron gas detector simulations including: gas detector wall effects, inactive areas at the end of detector tubes, and effects of a preamplifier. We acknowledge that DRiFT is under active development, bug reports and general questions and comments should be directed to Madison Andrews, madison@lanl.gov. This manual is divided into four parts: I) An overview of DRiFT, including how to obtain and install the executable, II) A description of the detector physics related to scintillators available, III) a description of more general DRiFT features the user may find useful, and IV) a description of the test suite and examples made available with the code release.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Application of a Triple Bubbler Inside Molten Salt for Pyroprocessing Safeguards Purposes

The application of a triple bubbler system within molten salt environments, specifically a eutectic mixture of LiCl-KCl, is explored for nuclear safeguards purposes, focusing on nuclear material accountancy (NMA) and holdup accountancy in pyroprocessing techniques. Traditional holdup accountancy methods, which involve periodic sampling and lengthy lead times, are being supplemented by the development of actinide sensors using electrochemistry. However, these methods alone are insufficient to meet regulatory requirements set by agencies like NRC and IAEA. The triple bubbler device measures salt level, density, and surface tension simultaneously using three dip tubes of varying diameters and heights. This study investigates the accuracy and robustness of the triple bubbler in molten salt conditions at temperatures ranging from 450-550°C. The updated bubbler design, utilizing tantalum metal and larger tube geometry, demonstrated minimal plugging and maintained measurement accuracy within acceptable uncertainties: 0.611% for depth, 1.34% for density, and approximately 40% for surface tension. Results indicate that the triple bubbler system is effective for real-time, accurate measurements in pyroprocessing environments, making it a promising tool for ensuring compliance with nuclear safeguards and supporting nuclear non-proliferation efforts.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Passive and active neutron signatures of 233 U for nondestructive assay

The thorium fuel cycle is emerging as an attractive alternative to conventional nuclear fuel cycles, as it does not require the enrichment of uranium for long-term sustainability. The operating principle of this fuel cycle is the irradiation of 232 Th to produce 233 U, which is fissile and sustains the fission chain reaction. 233 U poses unique challenges for nuclear safeguards, as it is associated with a uniquely extreme γ-ray environment from 232 U contamination, which limits the feasibility of the γ-ray-based assay, as well as more conservative accountability requirements than for 235 U set by the International Atomic Energy Agency. Consequently, instrumentation used for safeguarding 235 U in traditional fuel cycles may be inapplicable. It is essential that the nondestructive signatures of 233 U be characterized so that nuclear safeguards can be applied to thorium fuel-cycle facilities as they come online. In this work, a set of 233 U 3 O 8 plates, containing 984 g 233 U, was measured at the National Criticality Experiments Research Center. A high-pressure 4 He gaseous scintillation detector, which is insensitive to γ-rays, was used to perform a passive fast neutron spectral signature measurement of 233 U 3 O 8 , and was used in conjunction with a pulsed deuterium-tritium neutron generator to demonstrate the differential die-away signature of this material. Furthermore, an array of 3 He detectors was used in conjunction with the same neutron generator to measure the delayed neutron time profile of 233 U, which is unique to this nuclide. These measurements provide a benchmark for future nondestructive assay instrumentation development, and demonstrate a set of key neutron signatures to be leveraged for nuclear safeguards in the thorium fuel cycle.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Assessing Cognitive Impacts of Errors from Machine Learning and Deep Learning Models: Final Report

Due to their recent increases in performance, machine learning and deep learning models are being increasingly adopted across many domains for visual processing tasks. One such domain is international nuclear safeguards, which seeks to verify the peaceful use of commercial nuclear energy across the globe. Despite recent impressive performance results from machine learning and deep learning algorithms, there is always at least some small level of error. Given the significant consequences of international nuclear safeguards conclusions, we sought to characterize how incorrect responses from a machine or deep learning-assisted visual search task would cognitively impact users. We found that not only do some types of model errors have larger negative impacts on human performance than other errors, the scale of those impacts change depending on the accuracy of the model with which they are presented and they persist in scenarios of evenly distributed errors and single-error presentations. Further, we found that experiments conducted using a common visual search dataset from the psychology community has similar implications to a safeguards- relevant dataset of images containing hyperboloid cooling towers when the cooling tower images are presented to expert participants. While novice performance was considerably different (and worse) on the cooling tower task, we saw increased novice reliance on the most challenging cooling tower images compared to experts. These findings are relevant not just to the cognitive science community, but also for developers of machine and deep learning that will be implemented in multiple domains. For safeguards, this research provides key insights into how machine and deep learning projects should be implemented considering their special requirements that information not be missed.

97 MATHEMATICS AND COMPUTING↗

Regressing Nuclear Reactor Power Level Using Low-Cost Sensor Network Data

Multisensor networks deployed at nuclear facilities can be leveraged to collect data used as inputs to machine learning models predicting nuclear safeguard relevant information. This work demonstrates an application of this idea by regressing nuclear reactor power levels, a key indicator for nuclear safeguard verification, at the McClellan Nuclear Research Center using data collected by five Merlyn multisensor platforms with LASSO and LSTM models. This work also demonstrates the use of Leave One Node Out to measure the importance of each multisensor for this regression problem providing insight into model explainability and allowing inferential hypotheses about the nuclear facility to be made. This work can be used as a starting point for future development of methods for regression on reactor power levels at nuclear facilities using multisensor network data.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Development of a Neutron List Mode Collar (LMCL) and a List Mode Response Matrix Analysis Concept

This report was prepared for the Safeguards Program of the US Department of Energy’s (DOE’s) National Nuclear Security Administration (NNSA), Office of Defense Nuclear Nonproliferation Research and Development (DNN R&D). The report presents the development of the neutron nondestructive assay system, the List Mode Collar (LMCL) for the project OR16-List Mode for Collar-PD1La “List Mode Response Matrix for Advanced Correlated Neutron Analysis for Nuclear Safeguards.” The new list mode electronics developed under this project, and a spatial analysis concept called the List Mode Response Matrix are also described in this report. Analysis algorithms based on classification methods are published in a separate report. This research addresses the need to expand the capabilities of current nondestructive assay systems used for nuclear safeguards applications and considers the sustainability of safeguards technologies by the development of a “retrofit” concept using electronics based on modern standards. Furthermore, employing list mode data acquisition enabled the development of a spatial analysis concept and empirical measurement of a spatial response not previously used for safeguards neutron counting applications or measured in a traditional neutron collar detector and, therefore, provides new capability.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Safeguards Material Control And Accountancy Considerations For Molten Salt Reactors

Molten salt reactors are a class of nuclear reactor designs with features and operational characteristics that vary significantly. Variations in design features include the physical, chemical, and isotopic composition of fresh and irradiated fuel, neutron energy spectrums, breeding ratios, and the design’s plans for chemical processing. Specific designs within these variations affect the material control and accountancy approaches implemented by both domestic and international nuclear safeguards. This paper identifies safeguards-relevant design features for molten salt reactors and describes how each feature might influence both domestic and international nuclear safeguards implementation. Additionally, this paper describes two potential general categories of material control and accountancy approaches that may be appropriate for molten salt reactors: a black box material-balance approach with measurements on the feed and waste streams combined with robust containment and surveillance on the nuclear material within the reactor or an approach that aims to quantify the nuclear material throughout the reactor (i.e., a process monitoring approach). This paper describes the benefits and challenges of these approaches to meet technical safeguards objectives and identifies gaps in current technologies.

Hogue, Karen↗

Inspecta Technical Report

Sandia National Laboratories (SNL) is in the process of creating Inspecta (International Nuclear Safeguards Personal Examination and Containment Tracking Assistant), an Artificial Intelligence (AI)-powered smart digital assistant (SDA) with robotic capabilities, aimed at enhancing the effectiveness, efficiency, and safety of international nuclear safeguards inspections. This innovative tool is designed to assist inspectors on-site by supporting or automating tasks that are typically mundane, hazardous, or susceptible to errors. In 2021, the development team established the specifications for Inspecta by analyzing International Atomic Energy Agency (IAEA) documents and consulting with former IAEA inspectors and subject matter experts. This process involved aligning in-field inspection tasks with existing commercial or open-source technologies to outline a roadmap for the initial prototype of Inspecta, while also identifying areas needing further research and development. From 2022 – 2024, the focus has shifted to integrating a critical inspection activity, the examination of seals, into an early version of Inspecta. This has involved developing both the software and hardware capabilities necessary for this task. This report outlines the ongoing advancements in Inspecta's functionalities, specifically those supporting the seal examination process.

97 MATHEMATICS AND COMPUTING↗

Inspecta Technical Report

Sandia National Laboratories (SNL) has developed Inspecta (International Nuclear Safeguards Personal Examination and Containment Tracking Assistant), an AI-powered smart digital assistant (SDA) equipped with robotic capabilities. This innovative tool aims to enhance the effectiveness, efficiency, and safety of international nuclear safeguards inspections. Inspecta is designed to assist inspectors on-site by supporting or automating tasks that are often mundane, hazardous, or prone to errors. In 2021, the development team established the specifications for Inspecta by thoroughly analyzing International Atomic Energy Agency (IAEA) documents and consulting with former IAEA inspectors and subject matter experts. This process involved aligning in-field inspection tasks with existing commercial and open-source technologies, thereby creating a roadmap for the initial prototype of Inspecta and identifying areas requiring further research and development. From 2022 to 2025, the focus shifted to integrating a critical inspection activity—the examination of seals—into an early version of Inspecta. This phase has involved the development of both software and hardware capabilities essential for this task. This report outlines the advancements in Inspecta’s functionalities, particularly those that support the seal examination process.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Computational Modeling and Simulation for Nonproliferation: The History (and Present) of Monte Carlo and the MCNP(R) Code at Los Alamos [Slides]

The emergence of the Monte Carlo method as a research tool springs from work done at Los Alamos in the 1940s.Monte Carlo and the MCNP Code have been and continue to be developed at Los Alamos for many decades. From basic science in support of understanding nuclear interaction physics to global security applications, application uses of the code are extensive. Recent R&D projects and code modernization efforts make the MCNP code a great tool for nuclear nonproliferation applications. In collaboration with nuclear safeguards experts, new training has just recently been developed to help new practitioners learn how to use the code for nuclear safeguards applications.

97 MATHEMATICS AND COMPUTING↗

In situ liquid SIMS analysis of uranium oxide

Trace analysis of nuclear materials in solid particles collected in the environment or particles in liquid slurry generated in nuclear material manufacturing processes can pinpoint elemental, organic, and isotopic signatures of nuclear fuel cycle activities and processes. Such information can support nuclear safeguards programs by increasing our ability to detect undeclared nuclear materials, routine activities for safeguarding at declared facilities, and illicit activities. However, trace radioactive material analysis in liquids and slurries is challenging using bulk approaches. For example, one drawback of sensitive analysis such as inductively coupled plasma mass spectrometry (ICP-MS) is that sample is consumed or destroyed as a result of the technical approach. We developed a vacuum compatible microfluidic interface to enable surface analysis of liquids and liquid-solid interactions using time-of-flight secondary ion mass spectrometry (ToF-SIMS). In this work, we illustrate initial results of liquid standards containing uranium using in situ liquid SIMS. Specifically a series of diluted uranium standards used for ICPMS analysis were studied and the limit of detection was estimated. Since the liquid SIMS analysis is almost nondestructive, the same sample can be analyzed by other more destructive approaches afterwards or saved for future references. Consequently, multimodal analysis is possible. Our results demonstrate that in situ liquid SIMS can be used as a new approach to analyze radioactive materials in liquid and slurry forms of relevance to the IAEA safeguards missions.

In situ liquid ToF-SIMS, uranium, limit of detecti↗

Puck and Puck/SAW Loop Seals (Final Report)

Tamper-indicating devices (TIDs), also known as seals, play a crucial role in various sectors including international nuclear safeguards, arms control, domestic security, and commercial products, by ensuring that monitored or high-value items are not accessed undetected. These devices do not block access but alert to unauthorized tampering. With adversaries' capabilities evolving, there's a pressing need for seals to advance in terms of effectiveness (e.g., better tamper indication and unique identification), and new technology can improve the efficiency of installation and verification. Passive loop seals, widely used in international nuclear safeguards to ensure that continuity of knowledge is maintained on declared items, face stringent International Atomic Energy Agency (IAEA) requirements that surpass those met by commercial products. The metal cup seal (Figure 1, left), a staple IAEA seal, is robust but requires significant resources for post-use verification – specifically, the seal’s unique identity can only be verified at IAEA headquarters after removal from facilities. Further, the seal has been in use for decades and seal types should periodically be replaced to counter adversarial efforts for defeating seals. In 2020, the IAEA outlined about 40 requirements for a new passive loop seal, aiming for in-situ verification, minimal external tool use, unique identification (UID), and clear tamper indication. In response, research and development efforts focused on creating a new passive loop seal that meets these criteria and in 2022 the IAEA announced the completion of the Field Verifiable Passive Loop Seal (FVPS) (Figure 1, right). Concurrently to the IAEA’s efforts, Sandia National Laboratories (SNL) and Oak Ridge National Laboratory (ORNL) designed, developed, and tested two seal versions – Puck and Puck/SAW, with Puck based on the IAEA’s requirements and including a novel visually-obvious tamper response, and Puck/SAW adding additional beneficial capabilities like the ability to receive a unique identifier from a standoff distance and monitoring the wire integrity. Puck/SAW was specifically designed and developed to address sealing applications in dry spent fuel storage facilities, where the number of sealed spent fuel containers results in heavy verification burden and inspector safety issues related to radiation exposure. These efforts are described in this Executive Summary.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Cooperative Research and Development Agreement (CRADA) NFE-18-07194 with TerraPower LLC (Final Report)

Because of the potential economic and safety benefits of the molten salt reactor (MSR) concept, development of several designs has been initiated around the world over the past decade. New international nuclear safeguards needs and verification challenges are likely to arise because of the commercial interests in MSRs and the number of MSR design variants. As a result, work was undertaken to explore the cross-cutting issues specific to the application of international nuclear safeguards (i.e., safeguards) to liquid-fueled molten salt reactors (LFMSRs). Through a public-private partnership, a report was developed that focuses on the TerraPower Molten Chloride Fast Reactor (MCFR) design that has received a funding award from the US Department of Energy (DOE), Office of Nuclear Energy. The report is intended to provide a preliminary analysis for a safeguards-by-design (SBD) effort to inform designers about how safeguards could be applied to LFMSRs by the International Atomic Energy Agency (IAEA).Although the report specifically focuses on the TerraPower design, the conclusions are applicable to the main design features of LFMSRs and can be used to extrapolate how existing IAEA safeguards measures for other fuel cycle facilities can be appropriately applied or modified. The report evaluates the appropriate safeguards approaches for LFMSRs, presents existing safeguards inspection technologies are still valid for LFMSRs, and identifies new challenges that will require novel measurement instruments to meet verification standards of the IAEA and the international safeguards regime. This document summarizes the results of the work performed under the full report developed as part of the Cooperative Research and Development Agreement (CRADA). This summary does not contain any protected CRADA information and is intended for public release.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Absorber Clamp for Microcalorimeter Decay Energy Spectrometry

Microcalorimeter Decay Energy Spectrometry (DES) is of interest to nuclear safeguards due to its ability to provide high precision isotopic compositions of nanogram-to microgram-scale samples of Pu and U and related daughter products. The DES method is able to record decay energy of each alpha-decay event in a sample that is embedded in a metal matrix (absorber) and thermally linked to a microcalorimeter detector. This work optimizes the DES technique used to thermally link the absorber and microcalorimeter detector element to allow for more rapid assembly and to increase detector performance and operating life. Optimized attachment methods are crucial for enhancing the viability of DES in high-sample-throughput facilities, such as those that support international nuclear safeguards measurements. Here, in this study, we designed and implemented a pressure-based absorber clamp and evaluated the performance of this new attachment method relative to pressed indium bond attachment. Results using the absorber clamp demonstrate a streamlined detector assembly procedure that minimizes accidental damage to detectors, as well as increasing detector pulse speeds by 57%. Spectral comparison shows the clamp preserves detector performance relative to indium attachment.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Nonproliferation and Arms Control Research and Development (NPAC R&D) [Slides]

NPAC R&D focus areas include: Advancing U.S. capabilities to detect and characterize nuclear weapon development activities globally, including material production, the movement of special nuclear materials and nuclear weapons, and the testing or use of nuclear weapons, Supporting the development and testing of policy options and technical capabilities for international nuclear safeguards, arms control / treaty verification, nuclear export controls, and nonproliferation initiatives consistent with U.S. Government goals and objectives to enable monitoring and verification, Utilizing uranium, lithium, and high explosives (HE) materials expertise to support national-level activities in nuclear forensics and nuclear detection technology testing and evaluation, Providing unique training and capacity-building programs, particularly with the Nuclear Detection and Sensor Testing Center (NDSTC), and Engaging internationally to promote nonproliferation and arms control norms and best practices through bilateral and multilateral work.

36 MATERIALS SCIENCE↗

Direct Uranium Isotopic Analysis of Swipe Surfaces by Microextraction-ICP-MS

The ability to directly measure uranium isotope ratios on environmental swipes has been achieved through a solution-based microextraction process and represents a significant advancement toward the development of a rapid method to analyze international nuclear safeguard samples. Here, a microextraction probe is lowered and sealed onto the swipe surface, and analytes within the sampling site (~8 mm2) are dissolved and extracted into a flowing solvent of 2% nitric acid (HNO 3 ). The mobilized species are subsequently directed into an inductively coupled plasma-mass spectrometer (ICP-MS) for accurate and precise isotope ratio determination. This work highlights the novelty of the sampling mechanism, particularly with the direct coupling of the microextraction probe to the ICP-MS and measurement of uranium isotope ratios. The preliminary method detection limit for the microextraction-ICP-MS method, utilizing a quadrupole-based MS, was determined to be ~50 pg of 238 U. Additionally, precise and accurate isotope ratio measurements were achieved on uranium reference materials for both the major ( 235 U/ 238 U) and minor ( 234 U/ 238 U and 236 U/ 238 U) ratios. While the present work is focused on directly measuring uranium isotopic systems on swipe surfaces for nuclear safeguards and verification applications, the benefits would extend across many applications in which direct solid sampling is sought for elemental and isotopic analysis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗