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At least 127 records · Page 7

Prototype Demonstration of Gamma- Blind Tensioned Metastable Fluid Neutron/Multiplicity/Alpha Detector – Real Time Methods for Advanced Fuel Cycle Applications

The content of this report summarizes a multi-year effort to develop prototype detection equipment using the Tensioned Metastable Fluid Detector (TMFD) technology developed by Taleyarkhan [1]. The context of this development effort was to create new methods for evaluating and developing advanced methods for safeguarding nuclear materials along with instrumentation in various stages of the fuel cycle, especially in material balance areas (MBAs) and during reprocessing of used nuclear fuel. One of the challenges related to the implementation of any type of MBA and/or reprocessing technology (e.g., PUREX or UREX) is the real-time quantification and control of the transuranic (TRU) isotopes as they move through the process. Monitoring of higher actinides from their neutron emission (including multiplicity) and alpha signatures during transit in MBAs and in aqueous separations is a critical research area. By providing on-line real-time materials accountability, diversion of the materials becomes much more difficult. The Tensioned Metastable Fluid Detector (TMFD) is a transformational technology that is uniquely capable of both alpha and neutron spectroscopy while being “blind” to the intense gamma field that typically accompanies used fuel – simultaneously with the ability to provide multiplicity information as well [1-3]. The TMFD technology was proven (lab-scale) as part of a 2008 NERI-C program [1-7]. The bulk of this report describes the advancements and demonstrations made in TMFD technology. One final point to present before turning to the TMFD demonstrations is the context for discussing real-time monitoring of SNM. It is useful to review the spectrum of isotopes generated within nuclear fuel during reactor operations. Used nuclear fuel (UNF) from a light water reactor (LWR) contains fission products as well as TRU elements formed through neutron absorption/decay chains. The majority of the fission products are gamma and beta emitters and they represent the more significant hazards from a radiation protection standpoint. However, alpha and neutron emitting uranium and TRU elements represent the more significant safeguards and security concerns. Table 1.1 presents a representative PWR inventory of the uranium and actinide isotopes present in a used fuel assembly. The uranium and actinide isotopes (chiefly the Pu, Am and Cm elements) are all emitters of alpha particles and some of them release significant quantities of neutrons through spontaneous fissions

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Accountability Tanks Calibration Data Analysis

MET-1 utilizes tanks to store plutonium in solution. The Nuclear Material Control & Accountability group at LANL requires that MET-1 be able to determine the amount of SNM remaining in solution in the tanks for accountability purposes. For this reason it is desired to determine how well various operators may read the volume of liquid left in the tank with the tank measurement device (glass column or slab). The accuracy of the measurement is then compared to the current SAFE-NMCA acceptance criteria for lean and rich plutonium solutions to determine whether or not the criteria are reasonable and may be met.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Imaging of Nuclear Weapon Trainers

The Configurable Muon Tracker (CMT) is an adaptation of the existing drift tube detector commercially 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. The CMT became operational in February 2013. Traditionally, cosmic-ray muon trackers rely on near-vertical trajectory muons for imaging. Since there are scenarios where imaging using vertical trajectory muons is not practical, NSTec designed the CMT specifically for quick configurability to track muons from any trajectory. The CMT was originally designed to be changed from vertical imaging mode to horizontal imaging mode in a few hours with access to a crane or other lifting equipment. In FY14, locations for imaging weapon trainers and SNM were identified and it was determined that lifting equipment would not typically be available in experimental areas. The CMT was further modified and a portable lifting system was developed to allow reconfiguration of the CMT without access to lifting equipment at the facility. This system was first deployed at Los Alamos National Laboratory’s W-division, where several trainers were imaged in both horizontal and vertical modes. Real-time images have been compared in both modes showing that imaging can be done in both modes with the expected longer integration time for horizontal mode. Further imaging and post processing of the data is expected to continue into early FY15.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Dual-Particle Imaging System with Neutron Spectroscopy for Safeguard Applications

A dual-particle imager (DPI) has been designed that is capable of detecting gamma-ray and neutron signatures from shielded SNM. The system combines liquid organic and NaI(Tl) scintillators to form a combined Compton and neutron scatter camera. Effective image reconstruction of detected particles is a crucial component for maximizing the performance of the system; however, a key deficiency exists in the widely used iterative list-mode maximum-likelihood estimation-maximization (MLEM) image reconstruction technique. For MLEM a stopping condition is required to achieve a good quality solution but these conditions fail to achieve maximum image quality. Stochastic origin ensembles (SOE) imaging is a good candidate to address this problem as it uses Markov chain Monte Carlo to reach a stochastic steady-state solution. The application of SOE to the DPI is presented in this work.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Fission Meter Information Barrier Attribute Measurement System: FY2018 Office of Nuclear Verification FNI/UKC Task 2 Documentation Package

The ORTEC Fission Meter is a neutron multiplicity detector developed by Oak Ridge, TN based Advanced Measurement Technology (AMETEK), ORTEC Division. Data analysis techniques developed for neutron multiplicity detectors allows determination of mass and multiplication of unknown objects of special nuclear material (SNM). This can be done based on the physics of fission neutrons with little or no a priori information about the object. The articulating panel design and “5-Mode Counter” neutron multiplicity data-acquisition hardware were licensed to ORTEC by Lawrence Livermore National Laboratory in 2005 based on a 2004 prototype. The “5-Mode Counter” development started in 2000 in order to produce a compact neutron multiplicity file containing the full neutron count timing distribution. Development of this hardware along with the prototype detector design continued through 2004. Photographs of the Fission Meter are shown in Figure 1. In 2011, the Lawrence Livermore National Laboratory developed a software-based information barrier (IB) for the Fission Meter to control transmission of some for potential use in treaty applications. This IB was extended over the next several years to include improvements to the algorithms, more automated processing, and list mode data acquisition and processing. This report provides design and operational documentation for the Fission Meter and the Information Barrier additions.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Final Technical Report: Imaging a Dry Storage Cask with Cosmic Ray Muons

The goal of this project is to build a scaled prototype system for monitoring used nuclear fuel (UNF) dry storage casks (DSCs) through cosmic ray muon imaging. Such a system will have the capability of verifying the content inside a DSC without opening it. Because of the growth of the nuclear power industry in the U.S. and the policy decision to ban reprocessing of commercial UNF, the used fuel inventory at commercial reactor sites has been increasing. Currently, UNF needs to be moved to independent spent fuel storage installations (ISFSIs), as its inventory approaches the limit on capacity of on-site wet storage. Thereafter, the fuel will be placed in shipping containers to be transferred to a final disposal site. The ISFSIs were initially licensed as temporary facilities for ~20-yr periods. Given the cancellation of the Yucca mountain project and no clear path forward, extended dry-cask storage (~100 yr.) at ISFSIs is very likely. From the point of view of nuclear material protection, accountability and control technologies (MPACT) campaign, it is important to ensure that special nuclear material (SNM) in UNF is not stolen or diverted from civilian facilities for other use during the extended storage.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Sensitivity Analysis and Uncertainty Quantification of the Feynman Y and Sm 2

Neutron multiplicity counting (NMC) experiments are frequently used to perform non-destructive assay (NDA) of special nuclear material (SNM) [2]. While the behavior of a critical or nearly critical system is well described by the mean count rate, which is the mean of the NMC distribution, the behavior of a highly subcritical system exhibits large fluctuation in time. Fission chains do not last long enough to overlap and thus the neutron population is relatively small with a large dispersion. The system behavior must therefore be described in terms of higher-order NMC distribution moments.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Stilbene Scintillator Detector Array and Data-Acquisition System for Active Interrogation

A large area Stilbene crystal detector array has been assembled and calibrated for use in active interrogation measurements. The array consists of 10 high-efficiency 4”x2” stilbene cells. The cells were grown by Inrad Optics using LLNL developed technology. The array can be used to detect multiple signatures of SNM items, both actively and passively. Prompt and delayed gamma rays as well as prompt and delay neutrons can be detected and counted separately. The array is coupled to the Mesytec MDPP-16 VME-based digitizer module for data acquisition. This module performs on-board pulse-shape discrimination of signals from the Stilbene crystal detectors. This data-acquisition module allows separation of neutron and gamma-ray events with a low demand on data transfer rates. In addition, the high-resolution timing (<100 ps) is suitable for correlated gamma-ray and neutron multiplicity counting. This report describes the construction and calibration of the system. We also discuss applications of the system as well as how the system is currently being utilized by end users.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Verification and Validation of Optimization of Replacement Portal Monitoring Replay Tools

The Los Alamos National Laboratory and the Johns Hopkins Applied Physics Laboratory (APL) are both developing optimization software to fulfill the objective of Phase III of the Replacement Portal Monitoring (RPM) Program for the Department of Homeland Security. The objective of the Phase III of the RPM Program is to conduct an evaluation of three RPM systems designed to enhance mission effectiveness, gain operational efficiencies, and to address emerging mission needs against the Countering Weapons of Mass Destruction (CWMD ) nuclear threat basis and special nuclear material (SNM) used in performance testing. As such this task involves the use of global optimization algorithms.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

Sensitivity Analysis and Uncertainty Quantification Applied to the Feynman Y and Sm 2

Neutron multiplicity counting (NMC) experiments are frequently used to perform non-destructive assay (NDA) of special nuclear material (SNM), but MCNPR© code simulations of the counting distribution that were performed by Miller have revealed over-calibration in the value of the Pu-239ν¯. Mattingly has demonstrated the procedure for deterministic calculations of the counting distribution moments and O’Brien implemented a first-order, adjoint-based sensitivity analysis (SA) methodology applied to the counting distribution moments. In this report, these techniques are used to apply SA/uncertainty quantification (UQ) to the Feynman Y and Sm 2 , which are ratios of the counting distribution moments. Sm 2 is less sensitive to the cross sections than Y and therefore has less variance due to covariance in the cross sections than Y .

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Novel Perovskite Semiconductors for the Detection of Special Nuclear Material

Special nuclear material (SNM) detection using portable, highly efficient detectors is of paramount importance to national security for treaty verification and nonproliferation monitoring. The most mature technology for neutron detection is the 3He proportional counter; however, despite its high efficiency and ubiquitous use, 3He detectors have significant drawbacks, including long absorption lengths, high voltage requirements, and dependence on the availability of 3 He. The goal of this project is to synthesize a novel, boron-based perovskite semiconductor crystals to create a more efficient and more portable neutron detector. This innovative material will lead to a significant decrease in power and size requirements with higher operating temperatures than other traditional solid-state detectors. Directly incorporating 10 B eliminates the need for a conversion layer and leads to high neutron absorption coefficients. In this seedling project, we successfully synthesized millimeter sized crystals using inverse temperature crystallization with sizes of 1.73 mm in length and 480 μm in thickness.

36 MATERIALS SCIENCE↗

Nondestructive Assay for Nuclear Safeguards [Slides]

The objective of safeguards is the timely detection of diversion of significant quantities of nuclear material from peaceful nuclear activities to the manufacture of nuclear weapons. Currently, the IAEA is working to achieve universal acceptance of the AP, safeguards-by-design, unattended monitoring & data integration, and state-level concept/approach. We are trying to verify special nuclear material (SNM) is where it should be, and in the proper amount.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

TA-55 Forensic Support Operations Cross-Training Exercise

As part of the annual FBI/LANL training schedule, a joint training exercise was conducted during the week of 10FEB2020 with FBI HEAT members and LANL Fissile Material Handlers (FMHs). The joint training exercise was conducted in a non-radiological area to reduce cost and ensure the test object would not be contaminated. The exercise test object was fabricated by LANL using surrogate materials to represent an object containing Special Nuclear Material (SNM). Working with Jim Blankenship and Kevin Swearingen, functional requirements of the test object included the following: unclassified, disassembly (to include screws), and moderately heavy. To meet the objectives, the test object was fabricated by welding a custom aluminum box (8” x 8” x 12”) with a lid which was secured by four (4) screws. The custom box housed a track and field shot put (16 lbs.) that was anchored by a hose clamp. The intent of the training was to disassemble the test object and conduct traditional forensic determinations on the parts. This lessons learned report documents all of the associated aspects related to the joint training effort.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Radiation-Induced Modifications in Copper Oxide Growth

Radiation-induced effects and their influence on oxidation processes were evaluated for their use as a forensic tool for special nuclear material (SNM). A beam of 10 MeV Au³⁺ ions was used to mimic the accumulation of microstructural damage from self-irradiation through the decay of radionuclides. Several copper samples were irradiated as suitable surrogate materials at 200 °C with a flux of 1x10¹² ions/cm·s to damage levels of 5, 10, and 15 displacements per atom (dpa). This corresponds to about 50, 100, and 150 years, respectively, of accumulated α-decay damage in a PuGa alloy assuming a damage rate of 0.1 dpa/year. After irradiation, all samples were exposed to an accelerated aging process induced by thermal treatment at 350 °C for 1 hour in air. This resulted in the growth of a mixed oxide layer (Cu₂O and CuO) which was characterized in detail using several complementary analytical techniques: Scanning Electron Microscopy, Raman spectroscopy, Synchrotron X-ray diffraction (transmission mode), and Grazing Incidence X-ray diffraction. The oxide layer growth of irradiated Cu at 350°C is distinctly modified as a result of the ion irradiation. Most notably, the growth of the CuO phase is suppressed with increasing radiation damage on the Cu substrate, and structural changes occurred in the Cu₂O phase. These results indicate that damage from self-irradiation over time can cause quantifiable modifications in the oxidation process of metals that could be harnessed for their use as a novel forensic tool.

36 MATERIALS SCIENCE↗

Isotopic analysis of plutonium measured with very thick absorbers and high-granularity spectra

FRAM is LANL-designed software designed to extract plutonium and uranium isotopic information from gamma ray spectra. This is an important capability for NEST and STAB; however, FRAM performance has been poor when applied to field data collected in these programs. FRAM Version 5 (commercially available) was fine-tuned and validated for laboratory quality measurements but not for measurements of the high-mass and heavily shielded SNM items encountered in NEST. FRAM is untested for spectra collected with high-granularity lower resolution instruments such as the new 8-MeV Detective-X favored by STAB or the new custom electrocooled systems coming into use for NEST. FRAM Version 6.1 (unreleased) has improvements in physics capabilities, and parameter sets may be adapted that are more specific to NEST and STAB, which is what we have attempted for this assignment. Thick shielding attenuates gamma rays profoundly, especially those at low energy, making them too weak to be measured. The missing low-energy peaks force the analysis to employ only the highest-energy peaks. We adapted FRAM 6.1 for analysis of plutonium spectra obtained with very thick Pb filters (a surrogate for NEST-type configurations). New parameter sets employing only very high energy peaks were created for the analysis. High granularity and low resolution make deconvolution of the 600-keV region particularly challenging, and we have worked to optimally extract information from this region. The results shown in this paper give high confidence that we are on the right track. We used a combination of real and synthetically-modified data. Remaining work includes testing the new software and parameters against genuine data collected with Detective-X and new NEST systems, but such datasets at the moment are unavailable. It also remains to develop and test parameter sets specific to uranium and the new detectors.

07 ISOTOPE AND RADIATION SOURCES↗

Mixed-Material Scintillators (MMSS Quarterly Report FY20Q2)

This project aims to invent, model, and prototype mixed-material scintillator systems (MMSSs), a new class of radiation detectors that use heterogenous internal structures of different scintillating materials to detect additional properties of radiation. These internal structures can be produced using additive manufacture (3D printing) of scintillator, a currently emerging application of additive manufacture technology. MMSSs combine the low cost and complexity of conventional scintillation detectors with capabilities currently only available in more expensive and complex detectors. By identifying promising MMSS designs, this project will enable a new class of detectors to meet DNN’s mission needs for SNM detection. This quarter, we delivered one the MMSS Particle-ID Modeling report, a major deliverable of this project. This report describes our results on simulations of the particle-ID (PID) class of detectors. We found that these detectors outperform competing approaches for neutron-gamma discrimination, neutron source pointing, and neutron spectroscopy. Further highlights of the report are described below. During this quarter, We alerted HQ to a change in schedule for the remaining simulations planned for this project: we plan to put off further simulation and reporting of the position-resolving (PR) detector class until July. This change in schedule has allowed us to go into additional detail in the PID work that is both very promising and motivates our upcoming proposal. The other active task in this project is prototyping 3D-printed scintillators with the aim of realizing the designs we’ve simulated. On that front, we had three focuses: measuring the light output, increasing the size of printed parts, and combining blue and green scintillators. We succeeded in measuring the light output, showing an output of 30% of commercial standard. This result leaves room for improvement but is within striking distance of where we need to be. We were on track to demonstrate a key requirement for increasing the size of parts and also to show combined green/blue prints before the laboratory moved to a Minimum Safe (MinSafe) Operations posture as a result of local Shelter In Place orders due to Covid-19.

42 ENGINEERING↗

Mixed Material Scintillator Systems (Quarterly Report FY20Q3)

This project aims to invent, model, and prototype mixed-material scintillator systems (MMSSs), a new class of radiation detectors that use heterogenous internal structures of different scintillating materials to detect additional properties of radiation. These internal structures can be produced using additive manufacture (3D printing) of scintillator, a currently emerging application of additive manufacture technology. MMSSs combine the low cost and complexity of conventional scintillation detectors with capabilities currently only available in more expensive and complex detectors. By identifying promising MMSS designs, this project will enable a new class of detectors to meet DNN’s mission needs for SNM detection.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Proposed guidance for preparing and reviewing a molten salt non-power production or utilization facility application

Development of non-power molten salt reactors (MSRs) are under consideration to further establish an MSR experience base, support the requirements of Title 10 of the Code of Federal Regulations (10 CFR) Section 50.43(e), and provide any additional analyses needed for development of a full-scale MSR. Guidance provided in this report is based on MSRs operating with liquid fuel (i.e., fuel dissolved within a molten salt). These reactors, unless owned by the DOE or DOD, will require licensing by the US Nuclear Regulatory Commission (NRC) staff. Standard review plan (SRP) guidance for large light water reactors (LWRs) is available in NUREG-0800, Standard Review Plan for the Review of Safety Analysis Reports for Nuclear Power Plants; Light Water Reactor (LWR) Edition. However, NRC staff observed that NUREG-0800 is very cumbersome to apply to non-power reactors “because of the great differences in complexity and hazards between non-power reactors and nuclear power plants.” Therefore, a program to develop performance-based guidance applicable to non-power reactors was initiated. In 1996, NUREG-1537, Parts 1 and 2, Guidelines for Preparing and Reviewing Applications for the Licensing of Non-Power Reactors, was published. Part 1, the format and content guide, suggests a uniform format for presenting information in non-power reactor applications that is acceptable to the NRC staff, but conformance with the format and content is not required. Part 2, the SRP, ensures the quality and uniformity of the staff review of an application. Unfortunately, the application guidelines and SRP do not provide adequate guidance for all advanced non-LWR technologies and applications. This discrepancy eventually led to the 2012 development of interim staff guidance (ISG) for NUREG-1537, which includes criteria for describing and reviewing aqueous homogeneous reactors (AHRs). Specifically, NUREG-1537 ISG, 2012 expanded the original document to address three areas: 1. updated criteria for heterogeneous non-power reactors, 2. criteria for licensing AHRs, and 3. criteria for licensing a Part 50-licensed isotope production facility. In 2015, the US Department of Energy (DOE) opted to build on the AHR NUREG-1537 ISG experience by performing a gap analysis of the guidance that would be used to license a non-power MSR. MSRs represent one of the advanced non-LWR technologies selected by DOE for development through a multiyear cost share award with Southern Company Services. Under this Advanced Reactor Concepts 2015 (DOE Advanced Reactor Concepts [ARC] 15) award program, the DOE tasked Oak Ridge National Laboratory (ORNL) to evaluate the guidance changes that the NRC may need to consider when licensing an MSR non-power reactor. ORNL staff, with support from Boston Government Services, LLC, focused on five system-related chapters in NUREG-1537 that were considered most relevant to inform the effort that would be required for a non-power MSR applicant. ORNL documented this review in a technical report, ORNL/TM-2018/834, Proposed Guidance for Preparing and Reviewing Molten Salt Non-Power Reactor License Applications (NUREG-1537). The report was subsequently shared with industry and the NRC. The 2018 review was limited in scope, focusing on key system chapters based on the expected significance of each chapter relative to expected differences in addressing advanced non-LWR technologies, specifically non-power MSRs, compared with heterogeneously fueled non-power reactors. In the ORNL report, proposed generic adaptations were suggested for the following NUREG-1537 chapters: Chapter 4, “Reactor Description”; Chapter 5, “Reactor Coolant Systems”; Chapter 6, “Engineered Safety Features”; Chapter 9, “Auxiliary Systems”; Chapter 11, “Radiation Protection Program and Waste Management” The inclusion of Chapter 11 in the previous review effort was intended to provide guidance for categorizing the waste-handling process for an MSR operating with homogenous fuel. The introductions from Parts 1 and 2 of the 2012 NUREG-1537 ISG provide guidance for the application and review of production facilities. After a period of operation, non-power MSRs with homogenous fuel will include gaseous and soluble fission products. The gaseous fission products will be collected and held for decay in an off-gas system. There might also be an initiative to polish or filter the soluble fission products in the fuel salt by some mechanical or chemical means. The treatment and handling of fission products in the non-power MSR fuel salt and the description of this process in the safety analysis report (SAR) must be very precise to avoid the waste treatment facility being construed as a co-located special nuclear material (SNM) fuel cycle facility (see Section 2.3 of this report). Subsequent to the release of ORNL/TM-2018/834, NRC staff expressed a desire to continue the regulatory gap analysis that was begun in that report. This would provide additional clarity and information addressed in certain sections of the original report, while also providing new guidance on certain topics not addressed in the original report. This revision would benefit the NRC staff reviewing applications involving non-power MSR designs and would help developers understand how the NRC staff might approach the review of such applications. The focus of this report is to provide infrastructure support to the NRC staff for the regulatory review of non-power MSRs.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗