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At least 37 records · Page 2

Absolute Branching Ratios of Prominent $γ$ Rays Following $α$ Decay of 233 U

The absolute $γ$-ray branching ratios (emission probabilities) for 19 prominent peaks in the $α$ decay of 233 U are reported with energies ranging from 97 to 366 keV. The branching ratios were obtained from $α-γ$ coincidence measurements, normalized to the $α$ singles. The high-purity 233 U material (> 99.98%) was separated from its decay products before preparation of a 4.74-mg/cm 2 uranyl nitrate foil with a 6-mm diameter. Furthermore, this is the first report on the absolute normalization of the branching ratios since 1984 and it is the only measure by $α-γ$ coincidences, where the $α-γ/α$ ratio removes several potential systematic biases. Overall, the results are consistent with the adopted literature, and they validate the quantities most relevant to the non-destructive assay of fissile 233 U material, which is relevant to the thorium fuel cycle and associated safeguards.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Configuration and impurity quantification of AmLi sources using radiography and gamma spectroscopy

This paper presents the non-destructive assay of two AmLi sources used for detector characterization and active interrogation at PNNL, identified as MRC-101 and MRC-103. First, a detailed description of the internal configuration of 2724-BT encapsulated MRC sources is established. X-ray radiographs of the AmLi sources are reported for the first time to verify the dimensions and orientation of the encapsulation. Notably, a density variation was observed as a contrast change across the height of the source cavities. Contrary to commonly made assumptions in literature, it is indirectly observed that the AmLi source/target material only occupies a portion of the source cavity. The intensity of the prompt gamma-rays resulting from the inelastic scatter of alpha particles on 7Li was used to calculate the mass ratios of LiH:AmO2. The gamma-ray spectra revealed the presence of numerous impurities in both source and target material (243Am, 237Np, 154Eu, 23Na, and 9Be). Neutron-gamma production ratios were applied to the intensity of the Doppler-broadened peaks from alpha-induced reactions with 7Li, 9Be, and 23Na to calculate neutron rates for both sources. A neutron/alpha production yield (derived in this work) was then related to the atomic concentration of these isotopes to find the approximate masses within each source. Ultimately, the AmLi source density was estimated with prompt gamma analysis based on partial source volumes as 0.45±0.08 g/cm^3.

DTRA, AmLi, neutron↗

Improved evaluation of safeguards parameters from spent fuel measurements with the Differential Die-Away (DDA) instrument

The Differential Die-Away (DDA) technique is a highly sensitive non-destructive assay method for characterizing and detecting the presence of fissile material within an item of interest. DDA utilizes a series of pulses from a neutron generator (NG) to actively interrogate an item of interest. The die-away time of the neutron population induced by this active interrogation and the integral of the total differential die-away signal can be used to characterize items such as nuclear waste drums and spent nuclear fuel assemblies. In this work, Los Alamos National Laboratory (LANL) conceptualized, designed, and fabricated a DDA instrument that was deployed for field test measurements at the Central Interim Storage Facility for Spent Nuclear Fuel (Clab) in Oskarshamn, Sweden. The instrument performed multiple static measurements at fixed locations and dynamic axial scans of 15 pressurized water reactor (PWR) and 10 boiling water reactor (BWR) spent fuel assemblies, collecting both passive and active measurement data. The static assays of the assemblies measured the differential die-away signal, die-away time, and total passive neutron emission rate to create calibration curves for the evaluation of assembly multiplication, burnup, initial enrichment, effective fissile mass, and total elemental plutonium mass. Each calibration curve was optimized by minimizing the relative root mean square error (RRMSE) of assembly assay results compared to declared assembly parameters. The same quantities were also measured with the axial scans, and the resulting data were applied in two ways: (1) in the creation of calibration curves to improve evaluation of the same safeguards parameters as static assays, and (2) for comparison to simulation. In most cases, across both PWR and BWR assemblies, axial scan data improved the estimation of the above parameters, quantified by decreasing the calibration curve RRMSE. These axial scan results demonstrate the ability of the DDA instrument and analysis method to characterize spent PWR and BWR fuel as well as, or better than, a static assay of the same assembly. Furthermore, the DDA instrument’s unique ability to obtain both active and passive data in a single, axial scan of an entire spent fuel assembly represents a more efficient and accurate way of assaying spent fuel for verification purposes. These results represent a significant advancement for characterizing spent nuclear fuel compared to current technologies.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Data-Driven Performance Optimization of Gamma Spectrometers With Many Channels

In gamma spectrometers with variable spectroscopic performance across many channels (e.g., many pixels or voxels), a tradeoff exists between including data from successively worse-performing readout channels and increasing efficiency. Brute-force calculation of the optimal set of included channels is exponentially infeasible as the number of channels grows, and approximate methods are required. In this work, we present a data-driven framework for attempting to find near-optimal sets of included detector channels. The framework leverages non-negative matrix factorization (NMF) to learn the behavior of gamma spectra across the detector and clusters similarly-performing detector channels together. Performance comparisons are then made between spectra with channel clusters removed, which is more feasible than brute force. The framework is general and can be applied to arbitrary, user-defined performance metrics depending on the application. We apply this framework to optimizing gamma spectra measured by H3D M400 CdZnTe (CZT) spectrometers, which exhibit variable performance across their crystal volumes. In particular, we show several examples optimizing various performance metrics for uranium and plutonium gamma spectra in non-destructive assay (NDA) for nuclear safeguards, and explore trends in performance versus parameters such as clustering algorithm type. We also compare the NMF + clustering pipeline to several non-machine-learning (ML) algorithms, including several greedy algorithms. Although, we find that the NMF + clustering pipeline tends to find the best-performing set of detector voxels, significantly improving over the unoptimized spectra, but that a greedy accumulation of spectra segmented by detector depth can, in some cases, give similar performance improvements in much less computation time.

Energy resolution↗

Radiation Monitoring for Volatilized Zinc Contamination Using Gamma-Ray Imaging and Spectroscopy

Gamma-ray imaging is a tool that has grown in importance in the applications of non-destructive assay (NDA) for radioactive survey and analysis of nuclear facilities. Imaging techniques have shown great promise in providing valuable information involving radioactive waste management and contamination prevention. For the application studied in this work, 65 Zn has been identified as a radioactive contaminant during tritium extraction. Due to the volatile nature of 65 Zn under the pressure and temperature changes during extraction operations, 65 Zn can easily travel through components of the extraction system as vapor, making it difficult to trap. Previous research involving the development of a filtration system showed that the 65 Zn can be trapped, mitigating product contamination. However, during the extraction process, direct analysis of the equipment to confirm that zinc contamination is trapped in the filter and has not spread to other components is impractical. Here, in this situation, the need to assay the location of the contamination with little-to-no interference with operations is vital. In this work, we demonstrate the use of a commercialized 3D position-sensitive CdZnTe (CZT) gamma-ray imaging spectrometer to provide analysis of the 65 Zn contamination. Onsite measurements during an extraction process are studied to assess the location and migration of the 65 Zn. The results obtained from real-time glovebox monitoring demonstrate the feasibility of gamma-ray imaging for localizing the contamination and providing a preliminary qualitative assessment that is intended to be used in future work quantifying the contamination build-up and activity over time.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Spectral Peak Enhancement by Combining Trusted Response Elements via Machine Learning (SPECTRE-ML) v0.8.0

SPECTRE-ML (Spectral Peak Enhancement by Combining Trusted Response Elements via Machine Learning) is a machine learning based program for finding optimal clusters of radiation detector segments (i.e., pixels or voxels) in order to improve spectral performance. It provides facilities for pre-processing and analyzing training datasets, running ML algorithms, and evaluating and visualizing outputs. SPECTRE-ML outperforms simpler ad-hoc segmentation methods such as uniform depth clusters, learning detector performance trends such as dead layers, edge effects, and gain shifts. Although extensible to arbitrary highly-segmented spectroscopic radiation detectors, SPECTRE-ML currently focuses on improving spectral performance in highly-segmented CdZnTe (CZT) detectors for International Atomic Energy Agency (IAEA) non-destructive assay (NDA) safeguards tasks.

Vavrek, Jayson↗

Magnetic Microcalorimeter Gamma Detectors with Ultra-High Energy Resolution. Final Report

The goal of this project was to build a commercially viable metallic microcalorimeter (MMC) g-spectrometer with an ultra-high energy resolution <50 eV for accurate non-destructive assay (NDA) of nuclear materials. Improved NDA simplifies and accelerates safeguards analyses in the nuclear fuel cycle and enhances capabilities to detect the diversion of nuclear materials for illicit purposes. High-resolution MMC g-spectrometers can also improve the accuracy of nuclear data that NDA is based on.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

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 ↗

Magnetic Microcalorimeter Gamma Detectors with Ultra-High Energy Resolution - (Final Report)

The goal of this project was to build a commercially viable magnetic microcalorimeter (MMC) γ-spectrometer with an ultra-high energy resolution <50 eV for accurate non-destructive assay (NDA) of nuclear materials. Improved NDA simplifies and accelerates safeguards analyses in the nuclear fuel cycle and enhances capabilities to detect the diversion of nuclear materials for illicit purposes. High-resolution MMC γ-spectrometers can also improve the accuracy of nuclear data that NDA is based on.

42 ENGINEERING↗

Fixed-Energy Response-Function Analysis with Multi-Efficiency (FRAM) Software, Version 6

Researchers at Los Alamos National Laboratory have developed FixedEnergy Response- Function Analysis with Multiple Efficiency (FRAM), a powerful software tool for gamma-ray spectrometry isotopic analysis. This tool leverages Los Alamos expertise in nuclear safeguards, radiation detection systems, and related analysis techniques. A household name in the non-destructive assay community for over two decades, FRAM determines a special nuclear material source's isotopic composition by analyzing gamma-ray spectra. Los Alamos researchers have released the latest version of FRAM that incorporates several updates to the 2013 major release of FRAM, Version 5.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Keeping LANL at the forefront of list mode capability for safeguards and MC&A [Slides]

Neutron based detection forms key capability to enable and support international and domestic nuclear safeguards and non-proliferation missions. Key stakeholders include International Atomic Energy Agency (IAEA), European Atomic Energy Community (EURATOM), regional safeguards inspectorates, domestic stakeholders. LANL has been historically a leader in development of Non-destructive Assay (NDA) instruments and associated data acquisition hardware and software.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Outline for Feasibility Study on Nuclear Material Accounting and Control Technologies for Pu Fuel Cycle Facilities under Decommissioning at Tokai Site [Slides]

DOE/NNSA and JAEA to conduct a feasibility study on nuclear material accounting and control needs and requirements for non-destructive assay (NDA) measurement of material unaccounted for (MUF) in waste streams at JAEA Tokai fuel cycle facilities during the decommissioning process. Under this study, both sides will exchange information, perform an assessment of needs and requirements, and develop joint recommendations for development of NDA systems at select facilities.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Automated Fissile Mass Estimation Python Script for the Advanced Experimental Fuel Counter (AEFC)

The Advanced Experimental Fuel Counter (AEFC) is a non-destructive assay (NDA) instrument developed to quantify the residual fissile mass in research reactor spent fuel assemblies. The system is installed in a spent fuel pool and measurements are acquired underwater. A calibration curve relates the totals and coincidence counting signal from active interrogation of the spent fuel assemblies to the fissile mass remaining in the fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

New NDA Methods for Thorium Fuel Cycle Safeguards (Mid-Project Report)

This project is developing new Non-Destructive Assay (NDA) safeguards techniques for emergent thorium fuel cycles based on Neutron Resonance Transmission Analysis (NRTA), which can assay 233 U and 235 U when they are present together in a sample with potentially high gamma-ray backgrounds from fission products and 232 U. Existing passive techniques face large challenges for this task so new active interrogation methods are needed. This effort is also exploring how gamma-ray signatures can complement NRTA for enhanced assayed performance. This project leverages an NRTA system being developed at PNNL in collaboration with MIT, which uses a commercially available deuterium-tritium neutron generator at short standoff (~2 m). We aim to assess the feasibility and performance of these new NDA techniques for the range of relevant samples in thorium fuel cycles. Key advancements described in this mid-project report include NRTA system design for thorium safeguards measurements, characterization of 233 U oxide powder at PNNL, a survey of detector technologies suitable for NRTA in high gamma background environments, successful preliminary demonstration of a quantitative isotopic estimation algorithm, and first NRTA measurements of a thorium sample.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

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↗

Safeguards Technical Objectives for Thorium Molten Salt Reactor Fuel Cycles

China, Denmark, France, India, Indonesia, the United Kingdom, and the United States, among others, are exploring commercial thorium fuel cycles for domestic power production and/or international export. For any thorium fuel cycle facilities built and/or operated in a non-nuclear weapon State with a comprehensive safeguards agreement, those facilities and any associated nuclear material would be subject to international nuclear safeguards by the International Atomic Energy Agency (IAEA). Thorium fuel cycle facilities offered for the application of safeguards under a voluntary offer agreement by a nuclear weapon State would also be subject to safeguards, if selected by the IAEA. Compared to uranium/plutonium fuel cycle facilities, thorium fuel cycle facilities are comparatively diverse from an inspection and accounting perspective, differing greatly in material type, form, and design from uranium/plutonium fuel cycle facilities and also from each other. Of these, the most complex thorium fuel cycles – and therefore likely the most challenging to the implementation of international nuclear safeguards – are those that include thorium molten salt reactors. With thorium fuel cycles approaching near-term commercial deployment timelines, it is imperative that the international nuclear safeguards community begins to think about how to adapt existing international nuclear safeguards concepts and approaches to thorium fuel cycles, as well as mitigate any gaps that may exist. This paper focuses on the development of recommended safeguards technical objectives for efficient and effective application of international nuclear safeguards measures (e.g., containment / surveillance, non-destructive assay, destructive assay, environmental sampling) to thorium molten salt reactors.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

IAEA Facility-Level Safeguards and Implementation and Advanced Verification Technologies

IAEA Facility-Level Safeguards and Implementation - This presentation is intended to introduce the audience to the application of international safeguards by the International Atomic Energy Agency at nuclear facilities around the world. It covers the State Level Approach, random statistical sampling processes, material balance area structure, non-destructive assay techniques, and inspection areas. Addition of advanced verification technologies for the IAEA

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Examination of Digital-Delay Rossi-$\alpha$ for 252 Cf-Driven Highly Enriched Uranium Using Organic Scintillators

Neutron noise techniques constitute several analysis methods applicable to non-destructive assay. One technique is the Rossi-α method to calculate the prompt neutron decay constant (α) or its inverse, the prompt neutron period (1/α), for assemblies of fissionable material. This work evaluates a high-data-throughput measurement at the National Criticality Experiments Research Center (NCERC) with organic scintillators measuring a subcritical assembly of highly enriched uranium (HEU) metal (93% 235 U). The assembly comprises hemi shells stacked together to form fully closed shells and is driven by a Cf source at the center. The assembly is a total of 59.85 kg HEU and a k eff of 0.99, according to MCNP6.2 KCODE simulations. Measurements were acquired with a three-by-four array of 5.08-cm-diameter by 5.08-cm-length trans-stilbene crystals 166 cm from the assembly center. Two types of coincident binning methods are used to build the Rossi-α distribution of coincident neutron detections: A) type 1 binning, also known as any-and-all forward time differences, and B) type 1 binning with a digital-delay technique that is analogous to Orndoff’s use of delay cabling in early Rossi-alpha measurements. Method B) disregards same-detector coincidences and once all nearest time coincidences are collected between all detectors after a trigger, a time delay of 0.75 µs is implemented. The measured prompt neutron decay constants for both techniques are calculated from single exponential fits and the two methods are compared. Method A) shows an apparent timing discontinuity near 500 ns time differences. This timing discontinuity interferes with the fitting method used to calculate the prompt neutron decay constant. Method B) mitigates the artificial timing discontinuity and removes the disagreement of the fit. Future work will model the time-dependent detector response to discern why this timing discontinuity occurs, discern how Method B) reduces the amplitude of this timing discontinuity, and apply this method to critical assembly measurements to ultimately confirm the recommendation to use Method B) for high-data-throughput measurements.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗