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All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Verification of Special Nuclear Material (SNM) using Active Well Coincidence Counter (AWCC) and a High Purity Germanium (HPGe) Detector

SNM verification can be accomplished via two methods i.e. destructive analysis (DA) or nondestructive analysis (NDA). The DA modes are much more accurate compared to NDA modes; nevertheless, the sample's physical integrity is destroyed in the process. Techniques such as ICP-MS, ID-ICP-MS, TI-MS are few examples of DA, where a bulk material is ground and mixed with a solution (some form of acid) to acquire a homogenous sample. In contrast, NDA modes utilize signals emitted by the sample such as gamma, neutrons, light, or heat to analyze samples under investigation. HPGe detectors are some of the most frequently used gamma detectors to assay SNM. However, in a high activity scenario it provides a large uncertainty and sometimes becomes unfeasible to measure low energy gamma rays. Meanwhile, neutron detectors are not affected by the gamma background, therefore they can be used in addition to the gamma detectors to verify total fissile mass ({sup 235}U + {sup 239}Pu) of SNM. The AWCC is one of the thermal neutron NDA systems developed at the Los Alamos National Laboratory (LANL). It consists of 42 {sup 3}He detectors to measure gross neutrons (singles), coincidence neutrons (doubles), higher order multiplicity counting (triples, quadruples, etc.). It can effectively operate in both active and passive neutron interrogation modes. It can utilize AmLi, AmBe, or {sup 252}Cf active interrogation neutron sources. It is used to verify declared fissile mass ({sup 235}U or {sup 239}Pu) present in SNM. Objectives: Calibrate HPGe and AWCC for lightly irradiated (with enough {sup 137}Cs gamma background) ∼93% enriched HEU fuels; Verify fissile mass ({sup 235}U +{sup 239}Pu) content using AWCC and HPGe; Model and benchmark AWCC in MCNP6. Neutron coincidence and multiplicity counting: Two or more neutrons are coincident if they are detected by the system within the specified gate window; In AWCC: Gate window is 128 μsec; Induced fission in fissile material such as {sup 235}U and {sup 239}Pu - emission of time correlated neutrons - Singles, Doubles, Triples, or Quadruples; No induced fission in non-fissile materials- no correlated neutrons - only singles. SNM can be verified with high accuracy and precision using gamma and neutron NDA instruments such as HPGe and AWCC. Interaction with thermal neutrons. Non-fissile atoms - do not emit correlated neutrons. Fissile atoms - emit correlated neutrons during induced fission events. The time correlated neutrons can be detected by using coincidence or multiplicity counters such as AWCC. Likewise, {sup 235}U produces 186 keV gamma peak that can be measured by a HPGe gamma detector. Counts under 186 keV gamma peak provide information about {sup 235}U content. Combining AWCC and HPGe results can provide better understanding of special nuclear material under investigation.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Measuring SNM Isotopic Distributions using FRAM

The first group of slides provides background information on the isotopic composition of plutonium. It is shown that 240 Pu is the critical isotope in neutron coincidence/multiplicity counting. Next, response function analysis to determine isotopic composition is discussed. The isotopic composition can be determined by measuring the net peak counts from each isotope and then taking the ratio of the counts for each isotope relative to the total counts for the element. Then FRAM (Fixed energy Response function Analysis with Multiple efficiencies) is explained. FRAM can control data acquisition, automatically analyze newly acquired data, analyze previously acquired data, provide information on the quality of the analysis, and facilitate analysis in unusual situations (non-standard energy calibrations, gamma rays from non-SNM isotopes, poor spectra (within limits)).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Use of Sources and SNM in COE Facilities

This procedure describes how to use Special Nuclear Material (SNM) and sources in order to perform measurements in a safe manner. The hazards and controls associated with these activities are addressed in this document.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2023

SNM Radiation Signature Classification Using Different Semi-Supervised Machine Learning Models

The timely detection of special nuclear material (SNM) transfers between nuclear facilities is an important monitoring objective in nuclear nonproliferation. Persistent monitoring enabled by successful detection and characterization of radiological material movements could greatly enhance the nuclear nonproliferation mission in a range of applications. Supervised machine learning can be used to signal detections when material is present if a model is trained on sufficient volumes of labeled measurements. However, the nuclear monitoring data needed to train robust machine learning models can be costly to label since radiation spectra may require strict scrutiny for characterization. Therefore, this work investigates the application of semi-supervised learning to utilize both labeled and unlabeled data. As a demonstration experiment, radiation measurements from sodium iodide (NaI) detectors are provided by the Multi-Informatics for Nuclear Operating Scenarios (MINOS) venture at Oak Ridge National Laboratory (ORNL) as sample data. Anomalous measurements are identified using a method of statistical hypothesis testing. After background estimation, an energy-dependent spectroscopic analysis is used to characterize an anomaly based on its radiation signatures. In the absence of ground-truth information, a labeling heuristic provides data necessary for training and testing machine learning models. Supervised logistic regression serves as a baseline to compare three semi-supervised machine learning models: co-training, label propagation, and a convolutional neural network (CNN). In each case, the semi-supervised models outperform logistic regression, suggesting that unlabeled data can be valuable when training and demonstrating value in semi-supervised nonproliferation implementations.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗
DOE OSTI2017

Muon Tracking to Detect SNM

The Configurable Muon Tracker (CMT) is an adaptation of the existing drift tube detector commerically available from Decision Sciences International Corporation (DSIC). NSTec engineered the CMT around commercially available drift tube assemblies to make a detector that is more versatile than previous drift tube assemblies.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

Developing a Th Resonance Ionization Scheme: for Future Use in Age Dating SNM by Resonance Ionization Mass Spectrometry

We report the development of a Th resonance ionization scheme (RIS) for analyzing Th isotopes by resonance ionization mass spectrometry (RIMS) to enable age-dating via the 230 Th/ 234 U inter-elemental pair. This report summarizes the work that completes the first of two tasks that are required for developing U-Th dating via RIMS at the Laser Ionization of Neutrals (LION) laboratory at Lawrence Livermore National Laboratory (LLNL). The first task involves choosing and vetting an appropriate Th RIS for the LION instrument and simultaneous U and Th analysis.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2024

High-Energy Laser Direct Strike Assessment for NIF CryoXNBS Snout and Naiad SNM Container

An experimental IPT performed two NIF shots as an assessment of the effect of a direct laser beam strike impact on the NIF CryoXNBS snout and Naiad container. Four aligned NIF outer cone beams at best focus, 42 kJ total, struck a four millimeter thick stainless plate. In the first shot, the struck plate was followed by a 1.75 mm gap and a 2.0 millimeter stainless plate to create a surrogate geometry for the current CryoXNBS snout and Naiad container. There was minor plastic deformation of the rear plate rear surface with no evidence of bulk failure. The second shot tested a layered glass-filled polycarbonate and titanium shield placed in the gap. Nondestructive assay was sufficient to metrologize the beam strike area and the damage induced to the NIF target assemblies.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Diversion Path Analysis: A Proposed Methodology to Develop an MC&A Approach for Liquid-Fueled Molten Salt Reactors

Nuclear material control and accounting (MC&A) is a critical element of both the US Nuclear Regulatory Commission (NRC) and US Department of Energy (DOE)’s domestic safeguards and security requirements. NRC licensees are required, under Title 10 of the Code of Federal Regulations (10 CFR) Part 74 to establish and maintain an MC&A program that captures and records the quantities and locations of special nuclear material (SNM) at the facility. Along with physical protection, MC&A is a key element of domestic nuclear material safeguards that enables the NRC to ensure that SNM is controlled and accounted for. SNM, per 10 CFR Part 74, refers to plutonium, 233 U, and uranium enriched in the isotope 233 U or 235 U, but does not include source material. Periodic physical inventories, coupled with material balance evaluations, are effective and demonstrated tools to account for and detect theft or diversion of SNM in facilities containing SNM in bulk material form (i.e., not in discrete, countable items). Historically in the United States, these types of facilities have included fuel fabrication, conversion, and enrichment facilities. In comparison, reactors have relied on item counting of assemblies and control of SNM while in containment (e.g., a sealed reactor pressure vessel) because, to date, reactor fuel has been in item form. In liquid-fueled molten salt reactors (MSRs), unlike traditional light water reactors (LWRs) or bulk facilities, bulk SNM quantities can change significantly during operation as a result of depletion and transmutation. This introduces challenges to the use of traditional periodic physical inventories and material balance evaluations to detect theft or diversion of SNM in reactors that use SNM in bulk material form. Liquid-fueled (i.e., salt-fueled) MSR facilities are MSRs that use SNM within a salt eutectic as the fuel. The SNM is in a bulk material form any time it is outside of fresh or spent fuel storage containers. Some examples of when SNM will be in bulk form in the facility are during addition of fuel to the reactor system, while fuel is circulating in operation, and while fuel is in a drain tank. Periodic physical inventories and material balance evaluations can likely be effectively applied to many portions of an MSR facility, including all areas where depletion and transmutation are not significantly changing the quantities of SNM within the control area. Within an MSR facility, this would include fresh fuel receipt and loading, waste streams that may contain SNM, irradiated fuel storage outside of the reactor core, and any irradiated fuel processing that may happen after SNM has been removed from the reactor. All of these process steps could rely on measurements of SNM quantities compared with documented inventories. Any discrepancies from predicted (i.e., book) inventories and measured inventories could be quantified as inventory differences, consistent with traditional MC&A guidance from the NRC (e.g., in NUREG-1065 Revision 2, NUREG-2159 Revision 1, and RG 5.29 Revision 2). Within the reactor system, additions and removals to the book inventory include depletion of the SNM (e.g., fission of 235 U), which complicates the use of physical inventories. SNM control, however, can also likely be effectively applied to detect theft of SNM throughout a liquid-fueled MSR facility. To complement these approaches, prior technical reports have identified that a diversion path analysis may be a useful, risk-informed, and performance-based tool to determine suitable elements of an MC&A approach for the reactor system within a liquid-fueled MSR facility.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2019

Photofission Validation Measurements for Active Interrogation Standards

Executive Summary PNNL has been developing technical standards for the detection of special nuclear material (SNM) in cargo containers using active interrogation approaches. Since the use of kilogram-scale quantities of SNM is impractical for standards testing, the work focused on designing surrogates that provided similar signature as the SNM. There are many active interrogation approaches to detect SNM; the standards development considered photofission, differential die-away and nuclear resonance fluorescence. Of these approaches, photofission currently carries the most interest. However, uncertainties in the photofission cross sections are as large as 50%, so that validation measurements are necessary to provide confidence that the surrogate will perform similarly to the SNM. This document describes approaches for conducting those validation measurements as well as provides a rough order-of-magnitude cost estimate for performing them. Photofission provides many observables for the detection of SNM. The standards development considered prompt neutrons, delayed neutrons and delayed gamma rays as possible detected particles. The surrogates, which consist primarily of depleted uranium (DU), were designed to reproduce the strength of these particles for a targeted quantity of 2 kg of HEU. Different surrogates are required for different measurement approaches because of the difference in cross section between 235 U and 238 U. For the standards validations, the relative strength of the detected particles for HEU and DU must be measured. To avoid measurements with kilogram-sized SNM, the validation approach is focused on two comparisons. In the first comparison, the relative rates for approximately 10 g samples of DU and HEU will be measured. This comparison will provide the basis for validating the relative strength of the detected particles for HEU and DU. In the second comparison, the relative rates for the approximately 10 g and 1 kg sample of DU will be measured. This comparison will enable the validation of secondary processes that occur after photofission that impact the measurement for kilogram-scale samples. For instance, for 2 kg of HEU, as much as 50% of the fission induced in the sample is induced from fission neutrons generated through photofission. There is a limited range of facilities in the U.S. that have both the necessary accelerator capability and the ability and willingness to handle SNM. Two such facilities, the Idaho Accelerator Center at Idaho State University and the Nuclear Engineering Program at the University of Michigan, have both expressed an interest in participating in such measurements. Both would need to amend their licensing to handle the 10 g of HEU proposed for these measurements. The rough order-of-magnitude cost estimate for all three validation measurements is $1.1M, spread over three years. Each of the three measurements could be performed separately, at approximately one-third of that cost. There are a number of critical assumptions in these cost estimate that will need to be confirmed before a more reliable cost estimate can be established. PNNL will manage the effort to ensure that the overall objective of the validation measurements can be achieved and will fabricate the 10 g samples of HEU and DU. Most the labor for the measurements will be provided by two collaborating universities as research opportunities for students. The successful completion of these validation measurements will reduce the uncertainties in the proposed standards from about 50% to 5%. The measurements would also provide some much-needed nuclear data on photofission.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

Comparison of active interrogation methods for source location in a scattering and absorbing medium, consisting of PGNAA, and an AmBe quasi-forward biased directional source

Source location of Special Nuclear Material (SNM) encompassing 95% 235 U and 239 Pu is identified by utilizing a directional source from Patent No: US20190013109A1 using Prompt Gamma Neutron Activation Analysis (PGNAA) and neutron spectroscopy simulated with Monte-Carlo N-Particle transport 6.2 (MCNP). BC-408, HPGe, LaBr 3 detector arrays were used to identify the location of the SNM using total counts incident on each detector, and PGNAA photopeaks from HPGe and LaBr 3 detector arrays in a polyethylene shield. The conducted simulations varied the volume and location of the SNM in the MCNP input files to observe how the source location method behaved. PGNAA photopeaks used for source identification include 61 keV from fission, 2.223 MeV prompt gamma from hydrogen, 511 keV annihilation, and a single and double escape peaks from the prompt gamma interaction from hydrogen. The capabilities of each detector systems to acquire well resolved photopeaks with a 1% relative error or less, and total relative error for F4 and F8 tallies were less than 0.015% relative error. Source predictions of the SNM with uneven amounts of polyethylene shielding between the source and detectors was observed to overpredict and give invalid source location predictions. Source locations of the SNM with even amounts of polyethylene material between the source and each detector were found to be valid. With a 1 Ci 241 Am source activity, it was determined that 1630 s were needed to obtain the results for each detector system with the quasi-forward directional AmBe source. Coupling source and material identification together would increase acquisition time but would only require one system to determine.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Evaluation of a positron-emission-tomography-based SiPM readout for compact segmented neutron imagers

Gamma-ray emission from special nuclear material (SNM) is relatively easy to shield from detection using modest amounts of high-Z material. In contrast, fast-neutrons are much more penetrating and can escape relatively thick high-Z shielding without losing significant energy. Furthermore, fast neutrons provide a clear and unambiguous signature of the presence of SNM with few competing natural background sources. The challenge of detecting fast neutrons is twofold. First, the neutron flux from SNM are only a fraction of the corresponding gamma-ray flux. Second, fast neutrons can be difficult to differentiate from gamma rays. The ability to discriminate gamma rays from neutrons, combined with a neutron imaging capability, can in some situations enable the localization of SNM neutron sources distinct from background. With the developments of pulse-shape-sensitive plastic scintillators that offer excellent gamma-ray/neutron discrimination, and arrays of silicon photomultipliers combined with highly scalable and fast positron-emission-tomography (PET) multi-channel readout systems, field-deployable neutron imagers suitable for SNM detection might now be within reach. In this paper, we present a characterization of the performance of a recently available commercial PET-scanner readout, including its sensitivity to pulse-shape differences between fast neutrons and gamma rays, energy and timing resolution. Here, we find that, while the pulse-shape discrimination is achievable with stilbene, further improvement of the readout is required to achieve it with the PSD-capable available plastic scintillators.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Detecting and characterizing special nuclear material for nuclear nonproliferation applications

Abstract There is an urgent need for new, better instrumentation and techniques for detecting and characterizing special nuclear material (SNM), i.e., highly enriched uranium and plutonium. The development of improved instruments and techniques requires experiments performed with the SNM itself, which is of limited availability. This paper describes the findings of experiments performed at the National Criticality Experiments Research Center conducted using new instruments and techniques on unclassified, kg-quantity SNM objects. These experiments, performed in the framework of the Department of Energy, National Nuclear Security Administration Consortium for Monitoring, Technology, and Verification, focused on detecting, characterizing, and localizing SNM samples with masses ranging from 3.3 to 13.8 kg, including plutonium and highly enriched uranium using prototype detectors and techniques. The work demonstrates SNM detection and characterization using recently-developed prototype detection systems. Specifically, we present new results in passive detection and imaging of plutonium and uranium objects using gamma-ray and dual particle (fast neutron and gamma-ray) imaging. We also present a new analysis of the delayed neutron emissions during active interrogation of uranium using a neutron generator.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2017

Delayed Gamma-ray Spectroscopy for Safeguards Applications

The delayed gamma-ray assay technique utilizes an external neutron source (D-D, D-T, or electron accelerator-driven), and high-resolution gamma-ray spectrometers to perform characterization of SNM materials behind shielding and in complex configurations such as a nuclear fuel assembly. High-energy delayed gamma-rays (2.5 MeV and above) observed following the active interrogation, provide a signature for identification of specific fissionable isotopes in a mixed sample, and determine their relative content. Potential safeguards applications of this method are: 1) characterization of fresh and spent nuclear fuel assemblies in wet or dry storage; 2) analysis of uranium enrichment in shielded or non-characterized containers or in the presence of a strong radioactive background and plutonium contamination; 3) characterization of bulk and waste and product streams at SNM processing plants. Extended applications can include warhead confirmation and warhead dismantlement confirmation in the arms control area, as well as SNM diagnostics for the emergency response needs. In FY16 and prior years, the project has demonstrated the delayed gamma-ray measurement technique as a robust SNM assay concept. A series of empirical and modeling studies were conducted to characterize its response sensitivity, develop analysis methodologies, and analyze applications. Extensive experimental tests involving weapons-grade Pu, HEU and depleted uranium samples were completed at the Idaho Accelerator Center and LLNL Dome facilities for various interrogation time regimes and effects of the neutron source parameters. A dedicated delayed gamma-ray response modeling technique was developed and its elements were benchmarked in representative experimental studies, including highresolution gamma-ray measurements of spent fuel at the CLAB facility in Sweden. The objective of the R&D effort in FY17 is to experimentally demonstrate the feasibility of the delayed gamma-ray interrogation of shielded SNM samples with portable neutron sources suitable for field applications.

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2024

Special Nuclear Material Hold-up Measurement

Facilities that process special nuclear material (SNM) generally have a variety of equipment, shielding, and nearby radiation sources, which can pose challenges when performing nondestructive analysis (NDA) within the facility, as shown in Figure 1. In this figure, the left image features two individuals performing a holdup measurement of a large duct at a posting, utilizing a detector probe attached to a yardstick to reduce some aspect of the measurement uncertainty. Note that the distance to the holdup within the pipe from the posting cannot be accounted for. The right image similarly features several individuals guiding a holdup measurement of a ducting pipe several meters overhead, by attaching a detector probe to a long handle and lining that up with a posting on the outside of the pipe. SNM processing begets SNM holdup, and this difficulty with accurate NDA can result in unaccounted accumulation of SNM holdup within a process or area. Normal SNM processing operations can accumulate holdup within filters, pumps, pipes, ducts, other equipment, and facility support systems, as demonstrated by Figure 2. It is important for deactivation and decommissioning (D&D) gloveboxes and their ancillary equipment, material accountability, criticality safety, facility operations, waste management, radiation safety, and security to accurately characterize the location, composition, and quantity of this holdup to minimize these associated risks and potential diversion pathways. Current NDA techniques for assay of holdup are expensive, time consuming, and have high uncertainty.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗