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Demonstration of INCC6 for advanced list-mode data acquisition and analysis using ALMM

The International Neutron Coincidence Counting (INCC) software plays an important role in nuclear safeguards and nuclear material control and accounting (NMC&A) measurements. While the current version, INCC5, represents the traditional standard utilized by inspectorates as well as facilities and practitioners alongside shift register hardware, LANL has recently developed an upgraded version of the software, INCC6. INCC6 offers the same analysis tools as INCC5 while adding new capabilities including acquisition and analysis of list-mode data, recording and storage of list-mode data files, and an expanded set of advanced analysis tools that make use of the additional information available from list-mode data. Here, this paper presents the first demonstration of data acquisition and analysis using INCC6 and the Advanced List Mode Multiplicity Module (ALMM). The capability of INCC6 to perform live list-mode data acquisition and analysis is demonstrated for a variety of neutron sources with a range of neutron emission rates relevant for practical applications and validated against the results obtained with INCC5 and traditional shift register hardware. Advanced list-mode analysis tools introduced by INCC6, such as time-interval and coincidence matrix analysis, are also demonstrated. Finally, the capability of INCC6 to analyze list-mode data files is tested and validated against traditional shift register results using INCC5.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

A Better Method to Calculate Fuel Burnup in Pebble Bed Reactors Using Machine Learning

Burnup measurement is an important step in material control and accountancy (MC&A) at nuclear reactors, and may be done by examining gamma spectra of fuel samples. Traditional approaches rely on known correlations to specific photopeaks (e.g. 137 Cs) and operate via a standard linear regression method. However, the quality of these regression methods is limited even in the best case, and is significantly poorer at short fuel cool-down times, due to the elevated radiation background by short life-time isotopes, and self-shielding effect of the fuel. For practical operation of pebble bed reactors (PBRs), quick measurements (in minutes) and short cooling times (in hours) are required from a safety and security perspective. We investigated the efficacy and performance of machine learning (ML) methods to predict the burnup of the pebble fuel from full gamma spectra (rather than specific discrete photopeaks) and found a full-spectrum ML approach to far outperform baseline regression predictions in all measurement and cooling conditions - including in operational-like measurement conditions. We also performed model and data ablation experiments to determine the relative performance impact of our ML methods' capacity to model data nonlinearities and the inherent additional information in full spectra. Applying our ML methods, we found a number of surprising results, including improved accuracy at shorter fuel cooling times (the opposite of the norm), remarkable robustness to spectrum compression (via rebinning), and competitive burnup predictions even when using background signal only (i.e. explicitly omitting known isotope photopeaks).

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

An Assessment of the Safeguards Implications of Particle and Alloy Formation in MSRs

Molten salt reactors (MSRs) present unique challenges for applying safeguards measures and differ significantly from traditional nuclear reactors. Although the special fissionable materials within MSRs principally exist as dissolved species within the fuel salt, key actinides of interest may also be converted to solid phases including alloys and precipitated oxides via chemical and electrochemical reactions. These solid-phase components will complicate the nuclear material accounting and control (NMAC) approaches that have, so far, primarily targeted measurements of the liquid salt itself. For example, most of the proposed monitoring and characterization methods for MSRs are reliant on homogeneity of the salt and the ability to maintain accountable materials in solution. Solid deposits and particulates could invalidate the assumption of homogeneity and necessitate the use of new models and measurement tools to permit a full accounting of all nuclear material in an MSR. To address this, the likelihood of solids formation in MSRs, estimated the rate at which these solids could form, and assessed the monitoring tools that are available to account for the presence of these materials were examined. Specifically, three solid forming mechanisms were investigated, including (1) the accumulation of actinides within the MSR’s structural materials due to alloying, (2) the accumulation of actinides within noble metal fission product particulates, and (3) the generation of actinide oxides from interactions with salt impurities. These modeling-informed studies were completed with considerations to both fluoride- and chloride-containing salts. It was determined that, although measurable amounts of special fissionable material were expected to alloy with the structural elements and fission products, the predicted amounts were below levels considered as significant quantities (SQ) by the International Atomic Energy Agency (IAEA). However, it was determined that sufficiently large oxygen concentrations could potentially lead to significant quantities of special fissionable material being converted to solid oxide phases. As such, a comparative study of technologies that are commercially available to assist in monitoring and accountancy of this material was presented. Policy implications, design recommendations, and suggestions for follow-on experimental work were also presented to further assist reactor vendors in designing and controlling the fuel salt chemistry to address potential safeguards considerations.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Assessing the Impact of Increased Verification Measurements of Category III/IV Material Receipts

Revisions to the US Department of Energy (DOE) regulations for material control and accountability are expected to dramatically increase the number of verification measurements required upon receipt of nuclear material transfers. Material categories and types that were not routinely quantitatively measured upon receipt (Category III and IV) have been added to the more detailed regulations on shipments and receipts of nuclear materials. In anticipation of this change to the regulations, this project was initiated to identify measurement needs in the DOE complex with respect to performing these additional quantitative measurements. The results of surveying multiple DOE facilities to understand the scope of the impact and the potential measurement capability needs are presented.

Bean, Robert↗

Qualification and Re-Qualification of NDA Instruments

Non-Destructive Assay (NDA) instruments are a large component of nuclear material (NM) measurement at LANL. Nuclear Material Control and Accountability Group (SAFE-NMCA) personnel in the Safeguards Division are responsible for oversight of the instruments used for material accountability measurements. It is the responsibility of SAFE-NMCA to ensure that all instruments are operating as expected and can produce quality measurements to provide assurance that requirements of the DOE approved NMCA Plan are being met.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Study on Application of Distributed Network of Sensors with List Mode for NMAC Literature Review

Nuclear material accounting and control (NMAC) for nuclear security detects, deters, and resolves questions related to unauthorized removal (i.e. theft) or misuse of nuclear material. NMAC also serves as a key insider threat mitigation measure and aids in recovery of nuclear material that is missing. Effective nuclear security depends on NMAC for timely and accurate information about nuclear material types, quantities, and locations. Bulk nuclear material processing facilities, however, present unique challenges for effective NMAC due to the presence of large quantities of material in-process and the accumulation of residual material holdup within process equipment. These holdup accumulations can obscure accurate physical inventory taking and complicate efforts to resolve NMAC irregularities at the facility level. Bulk material monitoring systems often rely on material balance calculations and indirect measurement techniques, which may mask protracted theft of smaller amounts of nuclear material. These monitoring limitations have generated increased interest in continuous monitoring technologies, including distributed non-destructive assay (NDA) sensor networks capable of providing real-time or near-real-time measurement of material movement and accumulation within bulk processing environments. Recent advancements in distributed networks of NDA radiation detectors and sensing technologies provide an opportunity to address these limitations. Although such distributed sensor networks have been implemented in select facilities for IAEA Safeguards applications, their potential for supporting NMAC functions specifically tailored to nuclear security objectives remains largely unexplored. Furthermore, emerging list-mode data acquisition technologies have reached high technology readiness levels, enabling time-correlated detection of nuclear events across multiple temporal scales. These capabilities provide enhanced opportunities for accurate holdup measurement, continuous process monitoring, and improved detection of material theft or misuse over time. The increasing global expansion of civil nuclear power and development of related bulk material processing facilities, including those supporting high-assay low-enriched uranium (HALEU) and other advanced reactor fuel fabrication, further increases the need for advanced measurement and monitoring strategies for NMAC.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Domestic MC&A Recommendations for Liquid-Fueled MSRs

Investments by the US Department of Energy (DOE) are providing opportunities for vendors and developers of advanced reactor technologies to move toward experimental reactor systems, leading to commercial scale facilities. One facet of complementary research under the Advanced Reactor Safeguards program in the DOE Office of Nuclear Energy (NE-5) is motivated to assist vendors in licensing under the existing US (domestic) regulatory body’s federal regulations. This report provides concepts, approaches, and recommendations for liquid-fueled molten salt reactor (MSR) vendors to meet the material control and accountability (MC&A) and licensing requirements set forth by the US Nuclear Regulatory Commission (NRC) to possess and handle special nuclear material.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Delayed Neutron Temporal Signatures for Uranium Enrichment Measurement NA-241 SGTech (Final Report)

Nondestructive determination of uranium enrichment is a core capability for nuclear material accounting and control (NMAC) and safeguards verification measurements; however, traditional gamma spectroscopy-based techniques for enrichment measurement rely on significant assumptions of material composition and geometry, precluding their use in scenarios where a heterogeneous spatial distribution of enrichments is encountered. As an alternative, we are developing a technique to use delayed neutron temporal signatures for the measurement of uranium enrichment. Each uranium isotope has unique delayed neutron group yields, resulting in a unique delayed neutron decay time profile which can be analyzed to determine enrichment without the need for calibration sources. As part of this effort, we performed a series of measurement campaigns in which we used an active well coincidence counter (AWCC) retrofitted with commercial D-D and D-T generators to evaluate the operational characteristics of this method in response to a set of uranium enrichment and mass standards, as well as representative diversion scenarios in which either “concealed” enriched uranium is shielded by depleted uranium or declared enriched uranium is “hollowed out” and replaced with a central region of depleted uranium. A standard operating procedure and best practices were compiled to facilitate the use of delayed neutron-based enrichment measurements for international safeguards inspections.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Control Boundary Analysis for Liquid-Fueled Molten Salt Reactors

The US Nuclear Regulatory Commission (NRC) will likely require license applicants for liquid-fueled molten salt reactors (MSRs) with circulating fuel to submit a nuclear material control and accounting (MC&A) plan or provide a detailed MC&A program description for the facility. In liquid-fueled MSRs with special nuclear material (SNM) in bulk form (i.e., not in discrete items) and with rapidly changing quantities due to fuel transmutation and depletion, a novel MC&A approach is needed because traditional nuclear material accounting methods with material balance evaluations will not be sufficient. This report details the continued efforts carried out at Oak Ridge National Laboratory (ORNL) during FY 2025 to develop a distinct MC&A approach suitable specifically for domestic safeguards of the first-of-a-kind MSRs. These efforts are built on previous ORNL efforts reported in ORNL/SPR-2023/3181 and ORNL/SPR-2024/3555.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

New Capability at ORNL: High Precision Uranium Titration

Destructive analytical measurements establish a nuclear facility’s nuclear material inventory and inventory differences for Nuclear Material Accountancy and Control. A nuclear laboratory’s ability to perform accurate high-precision analytical measurements is key for tracking large inventories within a facility’s material balance areas and during production to track material movement through dynamic processes. For uranium, these measurements are made by using several established high-precision measurement protocols. These include isotope dilution mass spectrometry, gravimetry, and potentiometric titrations. Whatever measurement technique a nuclear lab chooses to use, reference materials (RMs) with certified attributes and accompanying uncertainties are used to calibrate measurement systems, and are the cornerstone for accurate results. In addition to calibration, RMs provide for metrological traceability, are used for method development and validation, and thus provide critical evaluations of the appropriateness and performance of analytical processes used. Evaluations may include validation that a method is fit-for-purpose, quantification of systematic and random biases, and the evaluation of long-term and short-term performance metrics. High-precision measurement techniques require that measured attributes be certified to a high degree of precision in the RMs used—ultimately, to a higher degree than that of the measurement technique itself. The US authority on the production of special nuclear material Certified Reference Materials is the NBL Program Office (NBLPO), formally known as New Brunswick Laboratory (NBL). The NBLPO is responsible for the sales and distribution of existing NBL certified reference materials (CRMs) and for the production of the next generation of nuclear RMs. To accomplish its mission, NBLPO is establishing key base capabilities within the DOE laboratory complex that formerly existed at the NBL laboratory. The Nuclear Analytical Chemistry (NAC) section within the Chemical Sciences Division (CSD) at Oak Ridge National Laboratory (ORNL) is currently working with NBLPO to set up laboratory and measurement capabilities to provide measurements and capabilities for production and/or recertification of existing and future CRMs for uranium assay. The NBL-developed high-precision titration (HPT) method is a critically-evaluated, extremely precise and accurate primary method utilized for the determination of uranium content in a variety of uranium materials. The HPT method, combined with detailed balance weighing protocols, provides for an analytical methodology that is unsurpassed in precision and one in which all sources of error have been evaluated, a requirement of CRM certification. HPT capability within the United States was lost with the closure of the labs at NBL. The NAC has been collaborating with NBLPO to stand up and demonstrate the capability to perform uranium assay via HPT at ORNL. HPT can produce results with an expanded uncertainty of approximately 0.01% for pure uranium compounds, with typical precisions of <0.006%. The major tasks required to stand up the method at ORNL were the refurbishment of a dedicated lab and equipment setup, procedure development, analyst training, establishing method-specific quality assurance, and qualification of an analyst to perform the method. This report summarizes these tasks, outlines the documents drafted, and gives the outcome of the qualification titrations.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Workshop on Improving Holdup Monitoring in the US

The characterization and quantification of nuclear deposits, or residual nuclear material retained in process equipment, generally referred to as holdup, continues to challenge nuclear processing facilities in DOE program areas such as nuclear criticality safety, material control and accountability, environmental management. The efficiency and effectiveness of nuclear operations in these facilities depends heavily on the results from nondestructive techniques designed to measure nuclear materials in situ. The traditional methods used to measure holdup were established more than 30 years ago and assume unrealistic conditions for most measurement cases. These blind, in situ measurements present unique challenges due to the following attributes: unique, non-ideal geometries; unknown deposit thicknesses; lack of representative calibration standards; large number of holdup deposit locations; and poor accessibility for many measurement locations. These difficulties and the poor assumptions made to handle them have resulted in measurement uncertainties that are often too large for many programs to effectively utilize. In an effort to address and identify solutions to the current holdup challenges facing the US nuclear industry, Oak Ridge National Laboratory hosted the Technical Workshop on Improving Holdup Monitoring in the US. The two-day workshop held August 21–22, 2019, was attended by 35 holdup measurement practitioners, program managers, stakeholders from US Department of Energy sites, the Nuclear Regulatory Commission, and representatives from commercial industry. The primary objectives were to identify critical elements of a successful and defensible holdup measurement program; identify technical challenges, needs, and potential improvements associated with measurement of holdup; and share best practices and lessons learned from recent accumulation events. Fourteen presentations were delivered on holdup topics including necessary elements for effective program management, measurement needs, emerging technologies and other measurement solutions, and lessons learned from recent events. These presentations highlighted best practices related to accumulation monitoring, considerations and proactive steps to facilitate holdup in new facility designs, imaging solutions to improve holdup assumptions, and new software developed in support of holdup measurements. Breakout sessions were also employed to determine additional needs and identify potential solutions to common holdup challenges. The primary discussions focused on causes and prevention of material accumulations, needs for uranium and plutonium measurements, and reduction of measurement uncertainty, all of which were explicitly identified as critical needs during the 2018 Workshop on Technical and Programmatic Needs for a Sustainable NDA Program for the US DOE.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Material Accountancy for Molten Salt Reactors: Challenges and Opportunities

The large upfront capital costs associated with new nuclear facilities is a substantial barrier to future growth. Facility retrofits to accommodate effective nuclear security can be expensive, particularly in facilities with large inventories of bulk nuclear material. The recent and sustained interest in advanced nuclear power presents the opportunity to implement material control and accountancy (MC&A) measures in the design phase to lower the possibility of costly retrofits.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Machine Learning Approaches for Nuclear Material Accounting Data from Irradiation and Reprocessing

We are currently exploring data analysis methods for their ability to strengthen the synthesis and evaluation of information generated within domestic and international safeguard regimes. Safeguard data typically includes rich heterogenous datasets amenable to advanced data analytics methods, such as machine learning. We have converted transactional data containing both numerical and categorical attributes from a domestic nuclear material control and accountability (NMC&A) system into a low-dimensional numerical structure via linear principal component analysis. This data representation allows for global structure discovery via cluster analysis, which can characterize the typical behavior of each of the primary types of transaction events. Furthermore, the structure of the top principal components captures the “typical behavior” of the data and is thus amenable to anomaly detection through statistical hypothesis testing. We explored this capability by generating erroneous permutations of the data and computing the Q-residual quantity increase associated with the information loss when these data are projected into the low-dimensional principal component analysis space representative of typical transactions.Future work will focus on identifying data transformations (e.g., graph networks) that more closely align with the inherent structure of these transactions to explain more salient information and disambiguate the underlying nuclear process—in this case, irradiation and reprocessing—from artifacts of NMC&A system transactional record keeping data.

Drescher, Adam↗

Simulation of Isotopic Concentrations and Gamma Spectra from Dynamic Fission Sources

A tool was developed to rapidly generate synthetic gamma-ray spectra to evaluate safeguards material control and accounting methods for liquid-fueled molten salt reactors. Molten salt reactor operations pose unique challenges to nuclear safeguards methods and protocols compared to deployed reactors designs (e.g., light water reactors). This research evaluates the use of gamma-ray spectroscopy to monitor fission product isotopic flow through a reactor model to understand expected operations and investigate changes to the spectra with material diversion scenarios. The large design space of molten salt reactors (e.g., liquid-fueled, liquid-cooled, online separations) could potentially lead to many measurement points within the reactor system. The developed analytical tool generates and evaluates synthetic gamma-ray spectra from dynamic reactor simulations by extracting isotopic inventory to generate source terms. An implementation in the Gamma Detector Response and Analysis Software (GADRAS) Application Program Interface (API) uses the source terms, a model of the reactor component, a detector response function, and measurement plan to quickly generate and analyze spectra. Prospective measurements are then evaluated in the more accurate but slower Geant4 simulations. Utilization of the developed modeling tool and analysis of the subsequent spectra enables optimization of collimation, shielding requirements, and expected count rates that are used to determine key measurement points in the modeled reactor design.

O'Brien, Sean↗

Improved plutonium and americium photon branching ratios from microcalorimeter gamma spectroscopy

Photon branching ratios are critical input data for activities such as nuclear materials protection and accounting because they allow material compositions to be extracted from measurements of gamma-ray intensities. Uncertainties in these branching ratios are often a limiting source of uncertainty in composition determination. Here, we use high statistics, high resolution - (60–70 eV full-width-at-half-maximum at 100 keV) gamma-ray spectra acquired using microcalorimeter sensors to substantially reduce the uncertainties for 11 plutonium ( 238 Pu, 239 Pu, 241 Pu) and 241 Am branching ratios important for material control and accountability and nuclear forensics in the energy range of 125 keV to 208 keV. Lastly, we show a reduction in uncertainty of over a factor of three for one branching ratio and a factor of 2–3 for four branching ratios.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Waste Compliance and Tracking System (WCATS) Version 3 Requirements Document

This document describes the end-user requirements for the Waste Compliance and Tracking System (WCATS) project in accordance with the WCATS Software Quality Management Plan, EPC-WMP-WCATSPLAN-001. The WCATS application shall support the generation, characterization, processing, and shipment of LANL radioactive, hazardous, and industrial waste. Regulatory drivers include RCRA hazardous waste, DOT shipping, NNSA nuclear material control and accountability, DOE nuclear safety, TSDF permit, and transuranic waste certification requirements. The system will utilize a task-based architecture that supports the spectrum of treatment, storage, disposal, administrative, and characterization based unit operations necessary to manage waste from cradle to grave. The application design shall readily accommodate new facilities, processes, workflow, signature requirements, and so forth, via end-user established metadata. WCATS will provide support for representing waste storage and disposal facilities, buildings, rooms, and grid layouts (x, y, z) to support waste and radioactive material inventory management. Nuclear material at risk (MAR), DOE hazard rating (e.g., Category II facility) compliance per DOE-STD-1027, and permit inventory requirements will be configurable for any storage or disposal facility, or waste operation, and the system will automatically evaluate and enforce those requirements. In addition, the application will support the characterization and management of the entire range of hazardous and radioactive wastes (TRU, MTRU, LLW, MLLW, hazardous waste, etc.) that might be colocated or processed at a permitted facility. Some capabilities not found in traditional systems include user-defined tank systems for liquid waste, user-defined work paths (i.e., sequence of operations), and an equipment subsystem for tracking the calibration, maintenance, and inspection of tools used to process waste, such as torque wrenches, scales, pH probes, etc. The application incorporates a desktop and mobile user interface as shown in Figure 1. The mobile interface supports field operations, such as waste item characterization, intra-facility transfers, internal and external audits, and shipment preparation and receipt.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Discrete-event Simulation Process Model for the Pyrochemical Processing of Plutonium at Los Alamos National Laboratory

The pyrochemical metal production operations that occur in the Plutonium Facility at Los Alamos National Laboratory perform plutonium purification with the aim to provide plutonium metal for a variety of defense- and non-defense missions within the National Nuclear Security Administration. The demands and constraints associated with the pyrochemical processing of plutonium are complex, making decision analyses challenging for program managers who require plutonium production for their mission applications. The construction of a discrete-event simulation process model is proposed to measure and report the process capacity, material throughput, equipment requirements, and dose accumulation for operators of the pyrochemical metal production operations. The process model, constructed in the ExtendSim™ software, will represent the cause-and-effect relationships between the pyrochemical processing environment and the process constraints, including criticality limitations, material control and accountability measures, chemical analysis requirements, and equipment availability. An accurate representation of the pyrochemical metal production process capacity through simulation modeling will be helpful to program managers in their efforts to forecast plutonium availability for mission applications. Furthermore, the proposed process model will be vital for future analyses that will measure the interactions between the pyrochemical metal production operations and the aqueous reprocessing operations and their ability to minimize transuranic waste disposal.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Application of Hybrid K-Edge Densitometry in Reprocessing Facilities

During reprocessing operations, accurately determining the elemental concentrations of uranium and plutonium is critical for nuclear security. Reprocessing facilities processes hundreds of tons of nuclear material annually, requiring accurate measurements to ensure effective nuclear material control and accountability. Hybrid K-edge densitometry (HKED) system combines K-edge absorption densitometry with x-ray fluorescence to measure actinide elemental concentrations with a low uncertainty. This system uses high-purity germanium gamma-ray detectors and advanced signal processing equipment to detect x-ray accurately. This document provides guidance on how to achieve effective performance from an HKED system for measuring uranium and plutonium concentrations in reprocessing facilities. It includes best practices for the setup and operation of an HKED system, while highlighting factors influencing uncertainties.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗