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Assessment of rare earth element fractionation in NIF implosions with radiochemically doped capsules

An ongoing experimental campaign at the National Ignition Facility (NIF) aims to measure neutron induced nuclear reaction cross–sections using radiochemically doped target capsules. Critical to this campaign is the ability to collect a representative sample of the reaction products using Solid Radiochemical Collectors (SRCs) fielded around the NIF chamber. The shot presented in this paper used a doped target capsule with a neopentane gas fill was to investigate the ratio of isotopes collected at three chamber angles. It was found that SRC samples of rare earth elements collected from NIF are representative of the ingoing dopant mix, thereby concluding that fractionation does not occur during a NIF implosion. This validates the doped capsule method for use in measuring neutron induced reaction cross-sections.

Capsule Doping↗

Weapon Material Program: FY24 Annual Report

The Weapon Material Program (WMP) framework was started in July of Fiscal Year (FY) 2022, along with other Mission Support organizations. The first year was about building the organization with the right people, identifying needs, and developing a vision for expectations. It was also a year to move forward with new equipment and technology for weapon material processes. With numerous improvements, WMP is building world-class systems for production, warehousing, and analytical testing. FY 2023 was a year of development. The WMP was a new organization defining its identity, its focus, and its mission. At the end of FY 2023, WMP evaluated its current position and its immediate needs along with its future goals. The entire organization set out on this FY 2024 journey to success. The lack of funding, staffing, and visibility dramatically impacted weapon material operations, testing, and qualifications. This neglect required numerous areas to be addressed and improvement plans to be developed and implemented. WMP processes, procedures, and overall business operations were dramatically in need of updating, revision, and formal documentation. This included all areas: technology, equipment, facility modifications/upgrades, and testing improvements. To ensure organizational improvement and forward momentum in FY 2024, WMP executed a multi-faceted strategic vision. Action items included the following: • Filling open positions with capable personnel who would contribute to a more robust organization • Establishing more formal operations and problem-solving techniques • Improving departmental procedures to align with expanding scope • Improving training • Establishing collaboration meetings with other departments/organizations • Focusing on the importance of identifying and mitigating concerns with At-Risk Materials (@RM) • Leading modernization eff orts for Blending and Packaging (B&P) We are on the verge of a transformational improvement in all of our processes in support of the mission. The following area achievements outlined in this report reflect the hard work toward achieving the goal of “being the material Subject Matter Experts in the nuclear enterprise”.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

Completion document for MRT 8824 - Upgrade NIF’s gaseous radiochemistry diagnostics (RAGS) to support weapons science

This milestone highlights the successful upgrade and deployment of the Radiochemical Analysis of Gaseous Samples (RAGS) system, which delivers high-quality measurements (<20% uncertainty) of activated gaseous species from NIF implosions. These measurements are critical for supporting Stockpile Stewardship Program (SSP) relevant platforms, including LANL’s Double Shell and LLNL’s Pushered Single Shell campaigns. The RAGS diagnostic technique enables analysis of short-range mixing in implosions using high-Z shells, which are otherwise inaccessible to conventional x-ray diagnostic methods. By facilitating the investigation of high-Z material mixing into fusion burn, this system provides essential data for quantifying and interpreting results in high-energy density (HED) experiments. This report details the physics motivation, diagnostic fundamentals, planned and enacted upgrade work, and the quantification of uncertainty for the upgraded system.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

ILLICIT TRANSIT INTERDICTION GLOBAL ANALYSIS

This study aims to enhance the security of radioactive materials during transport by analyzing commonalities in cargo thefts conducted by non-state groups such as thieves and terrorists. This research focuses on identifying patterns and trends in the methods used to steal high-value cargo, with the goal of applying these insights to improve transport security of radioactive materials. Key questions addressed include the frequency of specific tools, techniques, and insider involvement in thefts, as well as the use of weapons, electronic jamming equipment, and specialized tools. Findings will inform security design improvements and industry practices to mitigate vulnerabilities. The study involves a comprehensive review of literature and case studies, utilizing data sources from 2018 to 2023. Articles will be selected based on their relevance to thefts of valuable cargo in transit, with a focus on incidents involving non-state actors. The methodology will include statistical and inferential analysis to identify trends, with results visualized through pie charts, frequency analyses, and terrain maps. The discussion will highlight the implications of findings and provide actionable recommendations for strengthening security measures. Limitations such as data availability and reporting inconsistencies will be acknowledged. Suggestions for future improvements will be constructed using existing case studies and expert feedback. The study’s outcomes aim to raise awareness within the industry, inform policy decisions, and enhance security protocols for radioactive material transport. Metrics for impact include the potential publication of findings, presentations at conferences to raise awareness, and the subsequent actions taken by stakeholders based on the research. By identifying trends and vulnerabilities and suggesting improvements, this research contributes to preventing the illicit use of nuclear and radiological materials.

Zineddin, Dr. Z. [ORNL] (ORCID:0009000848740725)↗

Rossi-alpha measurements of fast plutonium metal assemblies using organic scintillators

The reactivity and the k-effective multiplication factor (k eff ) of a fissionable assembly are quantities of widespread interest. These values can be inferred from Rossi-alpha measurements of the prompt neutron decay constant (or the inverse:α -1 ). It has been shown that 3 He-gas proportional counter-based detection systems are insensitive to α -1 of fast assemblies (much faster than tens of microseconds). Therefore, it is of interest to investigate fast detection systems such as those based on organic scintillation detectors. In this work, an array of 12 cylindrical, 5.08 cm x 5.08 cm diameter trans-stilbene organic scintillators was used to measure five subcritical assemblies. One assembly was a sphere of approximately 4.5 kg of alpha-phase, weapons-grade plutonium (k eff = 0.773, α -1 = 11.84 ns) known as the BeRP ball encased in a thin stainless-steel clad. The other assemblies used the same encased sphere and 7.62 cm of iron, nickel, copper, or tungsten reflectors (k eff = 0.884, 0.916, 0.924, 0.939, respectively and α -1 = 36.60, 41.56, 49.60, 70.32 ns, respectively). Finally, this work (1) validates Rossi-alpha measurements with organic scintillators by demonstrating good agreement between measurements and simulations; and (2), demonstrates that organic scintillator-based systems are sensitive to α -1 on the order of 10–100 ns.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Radiological Handling and Containment Considerations in Support of an American Medical Isotope Producer

This work will discuss evaluation and design of new and modified facility level radiological containment, transfer, and handling systems in support of the United States’ American Medical Isotope Production Act. In the United States alone, Molybdenum-99 (Mo-99) is used as a precursor to locally generate its decay product, technetium-99m (Tc-99m), for use in approximately 40,000 medical procedures every day to detect cancer and heart disease. Currently, however, Mo-99 is primarily produced overseas and typically requires highly enriched uranium (HEU) which is classified as weapon -usable. This poses a serious security risk to the United States and, in 2012, Congress passed the American Medical Isotope ACT which aimed to cease all Mo-99 production that requires HEU and support American based companies who have found safer production methods. Through this effort, a system was designed and developed to access irradiated material in processing hot cells for ease of material introduction and removal in the confined area. The proposed solution uses a double-door design that allows for easy access to material while also providing shielding through a mechanically manipulated carousel. A system was also designed to transport irradiated materials from target reactors to a target receipt box using a rail guide system, pneumatic motor, and lead screw drive.

07 ISOTOPE AND RADIATION SOURCES↗

Small-scale production of bespoke accelerated aging plutonium alloy

Here, this study demonstrates the 100 g scale manufacture of a plutonium alloy that ages at an accelerated rate. The resulting alloy ages six times faster than typical weapons-grade plutonium due to the addition of 238 Pu. As a major innovation, the process involved using a partial direct oxide reduction technique. This method was achieved by developing a new, complex geometry stirrer using additive manufacturing to reduce the 238Pu oxide and efficiently incorporate it into weapons-grade plutonium metal. The material was then purified by molten salt extraction and electrorefining before being alloyed with gallium. The alloy was then cold-rolled and annealed in a homogenization heat treatment. The resulting disk was characterized by metallography and differential scanning calorimetry, and the impurity content was determined using analytical chemistry techniques. The results show that a homogeneous delta phase plutonium alloy was achieved with expected microstructure and minimal impurities. This study was also successful in changing the plutonium isotopic composition by incorporating additional 238 Pu to accelerate the effects of radiation damage. This enables researchers to study long-term aging phenomena in a reduced time frame, thus avoiding the need for large-scale material production and circumventing the limitations of using naturally aged, archived plutonium.

Aging theory↗

Literature Review of Documented Persistent Secondary Uranium Sources at DOE LM Sites

The U.S. Department of Energy Office of Legacy Management (LM) has the responsibility to protect human health and the environment at 101 legacy uranium sites across the nation by implementing long-term surveillance and maintenance requirements. Included in these responsibilities is to provide for the safe and environmentally sound disposal, long-term stabilization, and control of uranium mill tailings in a manner that minimizes or eliminates radiation health hazards to the public at 21 Uranium Mill Tailings Radiation Control Act (UMTRCA) Title I sites; 6 UMTRCA Title II sites; and 9 Comprehensive Environmental Response, Compensation, and Liability Act/Resource Conservation and Recovery Act sites. These sites are former uranium mills (processing sites), or sites with wastes from processing sites encapsulated in engineered disposal cells (disposal sites), or sites where components of atomic weapons were manufactured. During site characterization, groundwater contamination was often discovered and evaluated or modeled for future movement with the inclusion of uranium sorption in the groundwater plume. Much of this original work did identify uranium processing wastes as the original contaminant source. However, more recent work has identified the existence and influence of persistent secondary uranium sources that may prevent uranium in groundwater from attenuating as quickly as initial evaluations or modeling indicated. By understanding these processes, better decisions can be made to choose the appropriate remediation and closure strategies, identify long-term surveillance and maintenance activities, and more accurately estimate life-cycle costs. The purpose of this report is to summarize the literature available on documented persistence secondary uranium sources at LM sites as part of the Applied Studies and Technology Persistent Secondary Contaminant Sources Project.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Generalized rate theory for void and bubble swelling and its application to δ -plutonium

A rate theory for void and bubble swelling is derived that allows both vacancies and self-interstitial atoms to be generated by thermal activation at all sinks. In addition, they can also be produced by displacement damage from external and internal radiation. This generalized rate theory (GRT) is applied to swelling of gallium-stabilized δ-plutonium in which α-decay causes the displacement damage. Since the helium atoms produced also become trapped in vacancies, a distinction is made between empty and occupied vacancies. The growth of helium bubbles observed by transmission electron microscopy in weapons-grade and in material enriched with Pu238 is analyzed, using different values for the formation energy of self-interstitial atoms (SIA) and two different sets of relaxation volumes for the vacancy and for the SIA. One set allows preferential capture of SIA at dislocations, while the other set gives equal preference to both vacancy and SIA. It is found that the helium bubble diameters observed are in better agreement with GRT predictions if no preferential capture occurs at dislocations. Therefore, helium bubbles in δ-plutonium will not evolve into voids. Furthermore, the helium density within the bubbles remains sufficiently high to cause thermal emission of SIA. Based on a helium density between two to three helium atoms per vacant site, the sum of formation and migration energies must be around 2.0 eV for SIA in δ-plutonium.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Design and Materials of Reference Electrodes for Radioactive Waste Tank Service – A Literature Review

The Hanford site stores approximately 55 million gallons of radioactive and chemically hazardous wastes from the production of weapons materials. The wastes are stored in 177 underground, carbon steel storage tanks, 149 of these are single shell tanks (SSTs) and 28 of these are double shell tanks (DSTs). The DSTs provide critical retrieval and interim storage before the waste is vitrified in the Waste Treatment and Isolation Plant (WTP). The DSTs have been in service for 38 to 56 years and current plans indicate that WTP operations will be completed in 2075. Thus, the tanks will need to remain in service far beyond the initial 40-year life expectancy. For life extension of the tanks, effective corrosion control practices must remain in force. This effort includes direct measurements of the extent of corrosion (e.g., ultrasonic measurements and corrosion coupons) and electrochemical processes (e.g., linear polarization measurements).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Development of a High-Energy Neutron Sniffer and Subsequent Dose Quantification for High-Energy Particle Accelerator Shielding Surveys

The objective of this research is to design a portable neutron detector that is lightweight and responds to neutrons with energies of 20 MeV and greater. The instrument will be used as a ‘sniffer’ probe for identifying shielding weaknesses at high-energy particle accelerators and be paired with a plastic scintillator to quantify the high-energy neutron dose equivalent. The sniffer probes are two different sizes and comprised of either cesium iodide or sodium iodide, all doped with thallium, making a total of four detectors. The probes were calibrated to respond only to radiations with 8 MeV electron equivalent energy or higher, vastly reducing detector response from background and lower energy radiations. The sniffer probes were tested using californium- 252 and americium-beryllium sources, followed by high-energy (up to 800 MeV) neutron exposures at the Los Alamos Neutron Science Center Weapons Neutron Research (WNR) facility. The sniffer probes were then used to identify areas around the accelerator facility where elevated levels of high-energy radiation was present and the plastic scintillators were placed in these locations to determine the high-energy neutron dose equivalent. The dose equivalent is calculated by measuring the 12 C(n,2n) 11 C reaction, which has a 20.4 MeV neutron threshold. Two locations behind the WNR facility were identified with the probes and the dose equivalent rates from neutron energies above 20 MeV were calculated to be 1.24 mrem/h behind flightpath 30-left and 1.53 behind flightpath 30-right. Of the four sniffer probes, the 2-inch x 2-inch cesium iodide is the recommended probe for performing high-energy shielding surveys. The larger crystal size yields higher sensitivity at lower count rates and the more dense material increases the likelihood of interaction within the crystal.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Scoping Analysis of Pebble-Bed Reactors for the Destruction of the Transuranic Inventory of LWR Spent Nuclear Fuel

With the forecasted increase in the construction and operation of nuclear reactors, there will be a corresponding increase in the quantity of spent nuclear fuel (SNF) that requires long-term storage. In SNF, transuranic isotopes contribute the most to the long-term radiotoxicity of the fuel and pose a proliferation risk. One option that has been explored to address these issues is the removal of the transuranic isotopes from SNF and the conversion of these isotopes into transuranic fuel (TRU fuel). Here, this work sought to determine how effective a micro-modular Pebble-Bed High-Temperature Gas-Cooled Reactor (PB-HTGR); the 10-MW High Temperature Gas-cooled Test Reactor (HTR-10); and a salt-cooled small-modular pebble-bed reactor (PBR), i.e. the generic Fluoride-cooled High-temperature Reactor (gFHR), are at reducing the inventory of transuranic isotopes while still maintaining the intrinsic safety features of the PBR designs, such as negative temperature coefficients of reactivity. Optimized pebble designs utilizing TRU fuel were found for both reactors through the adjustment for the packing fraction of fuel in each pebble. The Axial Zone Equilibrium Modeling (A-ZEM) method was used in this work to help select the optimized pebble design. Once an optimized pebble design was selected and an equilibrium model was produced, the results from the deep burn (DB) HTR-10 and gFHR designs were compared to the results of two models from the literature. While both the DB gFHR and the DB HTR-10 were able to reduce the weapons-usable transuranic inventory, the performance of these reactors did not match that of the small-modular PB-HTGRs in the literature. Therefore, a need was identified for further refinement of the gFHR design using TRU fuel, as the results for this model were more promising than those of the DB HTR-10, which was strongly limited by the high leakage intrinsic to micro-modular PB-HTGRs.

Transuranic fuel↗

Panel Session 133: Integrating Economic Redevelopment and Workforce Transition Into DOE Site Closure Planning (R1.18)

This panel focused on post-closure impacts to the long-term site workforce and communities in DoE's approach to accelerated site cleanup and expedited reduction of long-term financial liabilities. At sites where Cold-War workers shifted from weapons production to the cleanup effort, a more holistic approach to the workforce transition Post-EM cleanup is needed. This holistic approach would include incentives for expedited closure, trade re-training, and a vision for future site commercial activities. The panel discussed the importance of the right workforce incentives that includes appropriate training for displaced workers so that they can be integrated into a next job. A key aspect of this discussion was to re-assess the current and future land use opportunities related to land re-use concepts. By re-arranging cleanup sequencing is it possible to divest land sooner than originally projected for productive commercial use hence reducing the DOE long-term liability and consequently increasing an economic soft landing for those Cold-War workers. Panelists with presentations: Integrating Economic Redevelopment and Workforce Transition Into DOE Site Closure Planning (Sean Todd); Sustaining, Growing and Re-Developing DOD/DOD Facilities and Assets (Jonathan Taylor)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Physical Sciences Vistas Issue 3 2021

In this issue, highlights of our contributions to mission operations include descriptions of the following. • How exact and scrupulous planning in concert with sophisticated science enabled a first-ever direct measurement of a radionuclide with a half-life as short as six days. The work, which included operations at the Los Alamos Neutron Science Centers (LANSCE) Weapons Neutron Research Facility and the Isotope Production Facility’s hot cell facility, is a boon for both astrophysics and weapons science. • An introduction to Christie Davis and her role in ensuring the Lab’s execution of simultaneous excellence. • A look at progress by AOT’s Target and Experimental Support Team in reclaiming long-dormant space in a radiological controlled area for new work improving target systems for the Lujan Center. • A story showcasing a cross-organizational effort to minimize the directorate’s legacy and environmental footprint. Staff from across the Lab joined together to ensure the safe and efficient disposal of Rocky Flats legacy waste stored in a transportainer at the Target Fabrication Facility. • How the Lab’s Utilities and Infrastructure experts collaborated with stakeholders in our directorate to safety execute preventive maintenance on the LANSCE mesa’s large electrical substation. The Safe Conduct of Research principles provided a common framework for the planning and process. • A description of the resources called upon and the procedures undertaken by MPA to inventory the division’s time-sensitive chemicals, including the careful and conscientious response of an alert team member when something seemed amiss.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

A holistic approach to the optimization of neutron beam transport at the LANSCE facility

An advanced neutron beam collimation system has been developed as part of an effort to optimize neutron beam transport at the Weapons Neutron Research (WNR) Facility, located within the Los Alamos Neutron Science Center (LANSCE). The goal of this work was to develop and demonstrate techniques to tailor neutron delivery in order to provide maximum available flux on sample with a specific beam profile, while simultaneously reducing unwanted background. A holistic approach was taken, upgrading the facility spallation target, facility metrology infrastructure, and flight path shutter insert to support the implementation of this advanced collimation system. Here, modern instruments and software were employed to conduct facility surveys, characterization of as-built geometry of critical components, 3D ray tracing and neutron transport calculations. Beam images and flux measurements were acquired after installation to evaluate the performance of the collimation system and to demonstrate consistent agreement with MCNP simulations which showed an 87% increase of flux on sample while providing suppression of background neutron impingement on the sample frame by 10 3 .

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Application of Neutron Multiplicity Counting Experiments to Optimal Cross-Section Adjustments

This paper presents the first application of model calibration to neutron multiplicity counting (NMC) experiments for cross-section optimization that is informed by adjoint-based sensitivity analysis (SA) and first-order uncertainty quantification (UQ). We summarize previous work on SA applied to NMC and describe notable modifications and additions. We give the procedure for first-order UQ and Bayesian-inference-based parameter estimation (PE). We then discuss model calibration applied to NMC of a 4.5-kg sphere of weapons-grade, alpha-phase plutonium metal (the BeRP ball) with the nPod neutron multiplicity counter. For the BeRP ball in bare and polyethylene-reflected configurations, we discuss the sensitivity of the first- and second-moment detector responses (i.e., first and second moments of the NMC distribution, respectively) to the cross sections. We describe the sources of uncertainty in the measured and simulated responses. Specifically, uncertainty in the measured responses is due to both random and systematic sources. Uncertainty in the simulated responses is due to the cross-section covariances. We describe in detail the adjustment to the cross sections and cross-section covariances due to the optimization. Due to the contribution of systematic uncertainties to the measured response uncertainties, the adjustment to the cross sections is similar in trend but larger in magnitude compared to that recommended by previous work. We compare the measured responses to responses simulated with nominal and optimized cross sections, demonstrating that the best-estimate cross sections produce simulations of NMC experiments that are more accurate with reduced uncertainty.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Design and commissioning of the Correlated Gamma-Neutron Array for sCattering (CoGNAC)

The Correlated Gamma-Neutron Array for sCattering (CoGNAC) is a dual $n$-$γ$ detector array fielded at the Weapons Neutron Research facility at the Los Alamos Neutron Science Center. Here, the detector array utilizes elpasolite detectors and liquid scintillators to perform measurements of neutron elastic and inelastic scattering cross sections and emitted particle angular distributions. This manuscript details the design and experimental setup of CoGNAC as well as some of the preliminary studies performed to select the elpasolite detectors deployed in the array. Examples of the analysis methods available to CoGNAC are given in the context of past CoGNAC measurements of neutron scattering reactions on 28 Si and 56 Fe.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The Teller–Ulam Innovation at 75: An Idea that Changed the World and Disputes over Credit

The 1951 Teller–Ulam breakthrough led to the 1952 invention of the hydrogen bomb and set the template for subsequent thermonuclear weapons designs that have played a pivotal role in geopolitics. In the years that followed, disputes arose as to how credit should be apportioned. This article surveys the claims made by Teller and Ulam, as well as by top U.S. scientists who were working with them on the H-bomb project at Los Alamos, drawing on many sources that are not widely available. It is hoped that these documented opinions of key scientific leaders (Bethe, Wheeler, Bradbury, Garwin, and so on), together with the cover page of the H-bomb patent, will be of interest to readers. The opinions vary widely, and even Teller and Ulam changed their assessments with time, becoming more convinced of their own dominant role as they aged. The average of the opinions is that Teller deserves about two-thirds of the credit and Ulam, one-third. While these disputes might detract from the elegance of scientific progress, they do show that advances occur from collaboration, competition, and varying lines of attack; indeed, the key contributors to this innovation might be better named as Teller–Ulam–Fermi–Konopinski–de Hoffmann.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗