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All sources NASA NTRS DOE OSTI

DOE OSTI2022

Suppressed thermal conductivity in hyperstoichiometric uranium dioxide controlled by phonon lifetimes

Thermal transport in nuclear fuels used for nuclear energy applications is directly tied to performance and reliability. Uranium dioxide (UO 2 ), one of the most important nuclear fuels, can accumulate excess oxygen atoms as interstitial defects, which significantly impacts thermal transport properties. In this study, thermal conductivities and inelastic neutron scattering (INS) measurements on UO 2+ x were performed at low temperatures (2–300K). The thermal conductivity of UO 2+ x (x = 0, 0.03, 0.04, and 0.11) is significantly suppressed compared to UO 2 except near the Néel temperature T N = 30.8 K, where it is independent of x. INS measurements demonstrate that the heat capacities and phonon group velocities of UO 2 and UO 2.08 are similar, and the suppressed thermal conductivity results from smaller phonon lifetimes. These perceptions advance our understanding of thermal transport properties in advanced nuclear fuels and guide safe and economic utilization of nuclear energy.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Ultrafast radiographic imaging and tracking: An overview of instruments, methods, data, and applications

Ultrafast radiographic imaging and tracking (U-RadIT) use state-of-the-art ionizing particle and light sources to experimentally study sub-nanosecond transients or dynamic processes in physics, chemistry, biology, geology, materials science and other fields. These processes are fundamental to modern technologies and applications, such as nuclear fusion energy, advanced manufacturing, communication, and green transportation, which often involve one mole or more atoms and elementary particles, and thus are challenging to compute by using the first principles of quantum physics or other forward models. One of the central problems in U-RadIT is to optimize information yield through, e.g. high-luminosity X-ray and particle sources, efficient imaging and tracking detectors, novel methods to collect data, and large-bandwidth online and offline data processing, regulated by the underlying physics, statistics, and computing power. We review and highlight recent progress in: (a.) Detectors such as high-speed complementary metal-oxide semiconductor (CMOS) cameras, hybrid pixelated array detectors integrated with Timepix4 and other application-specific integrated circuits (ASICs), and digital photon detectors; (b.) U-RadIT modalities such as dynamic phase contrast imaging, dynamic diffractive imaging, and four-dimensional (4D) particle tracking; (c.) U-RadIT data and algorithms such as neural networks and machine learning, and (d.) Applications in ultrafast dynamic material science using XFELs, synchrotrons and laser-driven sources. Hardware-centric approaches to U-RadIT optimization are constrained by detector material properties, low signal-to-noise ratio, high cost and long development cycles of critical hardware components such as ASICs. Interpretation of experimental data, including comparisons with forward models, is frequently hindered by sparse measurements, model and measurement uncertainties, and noise. Alternatively, U-RadIT make increasing use of data science and machine learning algorithms, including experimental implementations of compressed sensing. Machine learning and artificial intelligence approaches, refined by physics and materials information, may also contribute significantly to data interpretation, uncertainty quantification and U-RadIT optimization.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2023

High temperature gamma radiation-induced chromium redox chemistry via in situ spectroscopic measurements

Chromium ions can make their way into the primary coolant of nuclear power reactors from the corrosion of stainless-steel reactor components, decreasing the material's corrosion resistance and resulting in increased transport of further corrosion products. Despite these potential effects, the radiation-induced redox speciation of chromium ions in aqueous solution is not well understood, especially at the elevated temperatures experienced by reactor coolants. Here, in the present work, we report new experimental results demonstrating that in aerated aqueous solution, the radiolytic oxidation of Cr(III) to Cr(VI) occurs at pH 4, while the reduction of Cr(VI) to Cr(III) occurs at pH 2. The oxidation of Cr(III) is primarily attributed to the reaction of the hydroxyl radical (˙OH) with the Cr(OH) 2+ species, while the reduction of Cr(VI) is attributed to reactions involving the hydrated electron (e aq - ) and hydrogen atom (H˙). Additionally, the steady-state equilibrium yield of Cr(VI) from the gamma irradiation of pH 4 Cr(III) solutions decreased with increasing temperature (over a range of 37–195 °C). This observation indicates that the activation energy of the Cr(VI) reduction reactions is higher than that for the Cr(III) oxidation reactions, such that it becomes relatively more favorable at higher temperatures. Overall, these data are important for the development of complementary multiscale models for the prediction of metal ion speciation in high temperature radiation environments.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2021

Data supporting the article titled "Heterogeneous Multiphase Flow Properties of Volcanic Rocks and Implications for Noble Gas Transport from Underground Nuclear Explosions"

The submission is a Reproducible Research (RR) data archive that contains the supporting multiphase fluid flow and curve fitting results of the Vadose Zone Journal article titled: "Heterogeneous Multiphase Flow Properties of Volcanic Rocks and Implications for Noble Gas Transport from Underground Nuclear Explosions." The article's DOI number is the following: https://doi.org/10.1002/vzj2.20123. Please see the "Methods and Materials" section of the journal article and the ReadMe.txt in the RR_ARCHIVE folder for further details. Sandia National Laboratories is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International Inc., for the U.S. Department of Energy’s National Nuclear Security Administration under contract DE-NA0003525. SAND Number: SAND2021-3407 O.

mercury injection capillary pressure↗

DOE OSTI2020

Comparison of Modeled to Measured Spectra using MCNP and GADRAS to Benchmark and Contrast Modeling Limitations

The desire to improve nuclear material detection through portal monitors and other low resolution detectors has led to interest in benchmarking the performance of radiation transport codes. These codes can be used to generate a variety and quantity of spectra that may be cost prohibitive to measure directly. Particular characteristics of typical detection scenarios were isolated to compare the performance of radiation transport codes to laboratory experiments. These benchmark experiments were performed to validate simulations in a number of key areas. These experiments included high areal density configurations in both one- and three-dimensional configurations. In addition, off-angle measurements were conducted to investigate the impact of detector response assumptions on complex geometries, for example where an unknown source is not physically collocated with an apparent hot spot. Furthermore, by examining both simple shielding and backscatter configurations, isolation of the scatter emanating from the object and environmental background scatter contributions to the spectra could be elucidated. A series of experiments were performed in which the order of shielding layers and the thickness were evaluated to examine the ability of the simulations to address these variables. Experiments with increasing thickness of polyethylene around a neutron source also allows for examinations of the ability of the transport simulations to properly model n,γ reactions. Finally, depleted uranium (DU) measurements have more complicated spectra than the cobalt-60 and consequently allow for investigations into the ability of transport simulations to model self-shielding. In each case, the results of the experiments were compared to MCNP simulations to judge the performance of the code, as was done previously with GADRAS 18.7.9 simulations [7]. All of the benchmark measurements were taken with a liquid nitrogen cooled 140% high purity germanium (HPGe) detector with a bismuth collimator that had the front tin filter removed. The measurement location and detector configuration were subsequently used for all experimental configurations. The remainder of this report details the experimental measurements, Section 2 and the MCNP model, Section 3. Comparisons between the experimental results and MCNP-generated spectra are performed, Section 4. Section 5 compares the results obtained with MCNP with the previously reported results obtained with GADRAS [2]. Finally, Section 6 presents the conclusions.

61 RADIATION PROTECTION AND DOSIMETRY↗

NASA NTRS1989

Space radiation shielding strategies and requirements for deep space missions

Methods for estimating crew exposure to radiation and for evaluating shield requirements for spacecraft equipment and crew are examined. The development status for deterministic space radiation transport computer codes and models of their nuclear interaction inputs, which are useful for estimating the composition and thickness of shield materials, is discussed. The relation between shield thickness and exposures is studied. Estimates of deep-space shield requirements are proposed. It is noted that an assessment of input parameter uncertainties reveals that a factor of 2 uncertainty in predicted dose equivalent could increase shield thickness by an order of magnitude of more.

Townsend, Lawrence W.↗

NASA NTRS1992

Radiation health for a Mars mission

Uncertainties in risk assessments for exposure of a Mars mission crew to space radiation place limitations on mission design and operation. Large shielding penalties are imposed in order to obtain acceptable safety margins. Galactic cosmic rays (GCR) and solar particle events (SPE) are the major concern. A warning system and 'safe-haven' are needed to protect the crew from large SPE which produce lethal doses. A model developed at NASA Johnson Space Center (JSC) to describe solar modulation of GCR intensities reduces that uncertainty to less than 10 percent. Radiation transport models used to design spacecraft shielding have large uncertainties in nuclear fragmentation cross sections for GCR which interact with spacecraft materials. Planned space measurements of linear energy transfer (LET) spectra behind various shielding thicknesses will reduce uncertainties in dose-versus-shielding thickness relationships to 5-10 percent. The largest remaining uncertainty is in biological effects of space radiation. Data on effects of energetic ions in human are nonexistent. Experimental research on effects in animals and cell is needed to allow extrapolation to the risk of carcinogenesis in humans.

Robbins, Donald E.↗

NASA NTRS2011

Thermal Energy for Lunar In Situ Resource Utilization: Technical Challenges and Technology Opportunities

Oxygen production from lunar raw materials is critical for sustaining a manned lunar base but is very power intensive. Solar concentrators are a well-developed technology for harnessing the Sun s energy to heat regolith to high temperatures (over 1375 K). The high temperature and potential material incompatibilities present numerous technical challenges. This study compares and contrasts different solar concentrator designs that have been developed, such as Cassegrains, offset parabolas, compound parabolic concentrators, and secondary concentrators. Differences between concentrators made from lenses and mirrors, and between rigid and flexible concentrators are also discussed. Possible substrate elements for a rigid mirror concentrator are selected and then compared, using the following (target) criteria: (low) coefficient of thermal expansion, (high) modulus of elasticity, and (low) density. Several potential lunar locations for solar concentrators are compared; environmental and processing-related challenges related to dust and optical surfaces are addressed. This brief technology survey examines various sources of thermal energy that can be utilized for materials processing on the lunar surface. These include heat from nuclear or electric sources and solar concentrators. Options for collecting and transporting thermal energy to processing reactors for each source are examined. Overall system requirements for each thermal source are compared and system limitations, such as maximum achievable temperature are discussed.

Gordon, Pierce E. C.↗

DOE OSTI2022

Morphological-informed Thermal Property Prediction in the Engineering Domain

Using first-principle, atomic scale methods to predict thermal carrier (electron and phonon) behavior at nanoscale yields highly resolved thermal properties. Density functional theory simulations can model myriad effects on the transport of phonons and electrons (e.g., phonon and electron coupling, electron correlation, defect presence, carrier scattering), and yield thermal properties for small geometric domains such as thermal and electrical conductivity, or heat capacity. While these thermal properties are accurate in atomistic and nanoscopic systems, they must be scaled up to the microstructural domain to be a useful predictor for experimental basis, as the microscale is where myriad changes and physical phenomenon occur within a material (e.g., grain boundaries, precipitate aggregations, interfaces, defect clusters). My talk will discuss the necessity of thermal property predictions for nuclear fuels applications and more. Additionally I will discuss the necessity in developing multi-physics, multi-scale methods for future applications in predictions for not only nuclear fuels, but other materials applications.

36 MATERIALS SCIENCE↗

NASA NTRS2003

Radiation Transport Properties of Potential In Situ-Developed Regolith-Epoxy Materials for Martian Habitats

Mission crews in space outside the Earth s magnetic field will be exposed to high energy heavy charged particles in the galactic cosmic radiation (GCR). These highly ionizing particles will be a source of radiation risk to crews on extended missions to the Moon and Mars, and the biological effects of and countermeasures to the GCR have to be investigated as part of the planning of exploration-class missions. While it is impractical to shield spacecraft and planetary habitats against the entire GCR spectrum, biological and physical studies indicate that relatively modest amounts of shielding are effective at reducing the radiation dose. However, nuclear fragmentation in the shielding materials produces highly penetrating secondary particles, which complicates the problem: in some cases, some shielding is worse than none at all. Therefore the radiation transport properties of potential shielding materials need to be carefully investigated. One intriguing option for a Mars mission is the use of material from the Martian surface, in combination with chemicals carried from Earth and/or fabricated from elements found in the Martian atmosphere, to construct crew habitats. We have measured the transmission properties of epoxy-Martian regolith composites with respect to heavy charged particles characteristic of the GCR ions which bombard the Martian surface. The composites were prepared at NASA Langley Research Center using simulated Martian regolith, in the process also evaluating fabrication methods which could lead to technologies for in situ fabrication on Mars. Initial evaluation of the radiation shielding properties is made using radiation transport models developed at NASA-LaRC, and the results of these calculations are used to select the composites with the most favorable radiation transmission properties. These candidates are then evaluated at particle accelerators which produce beams of heavy charged particles representative in energy and charge of the radiation at the surface of Mars. The ultimate objective is to develop the models into a design tool for use by mission planners, flight surgeons and radiation health specialists.

Miller, Jack↗

DOE OSTI2022

Particle transport in Markov stochastic mixtures with spatial gradients

Markov geometries are a prototype class of stochastic media that are widely used to model complex disordered systems. In a series of recent works, we have shown that spatially homogeneous (but possibly non-isotropic) Poisson tessellations can be conveniently used in order to generate three-dimensional realizations of Markov media and thus characterize the features of particle transport e.g. in fragmented fuel elements following severe nuclear accidents or Rayleigh-Taylor turbulent mixing for inertial confinement fusion. In this paper we show that Poisson tessellations can be extended to take into account the presence of spatial gradients, which commonly occur in real-world applications due to material stratification. For this purpose, we will provide an explicit construction of spatially-non-homogeneous Poisson tessellations, fully characterize their statistical properties, and finally illustrate the behaviour of particle transport in such random media. (authors)

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2022

The Influence of Environment on Post-Detonation Chemistry and Debris Formation (Abbreviated Final Report: 20-SI-006)

Predicting, responding to, or interpreting the chemical record preserved in debris derived from nuclear events can be challenging due to chemical fractionation. Chemical fractionation is where different species of the evolving radionuclide inventory segregate and/or are lost from the system over the timescales of debris formation. Both historic data and recent research suggest that the interaction and character of the local environment may exert controls on chemical fractionation by influencing the cooling and evolution of the associated fireball as well as the composition of the vapor term and resultant speciation. Prior to this work, an integrated platform permitting dynamic and concurrent consideration of physical and chemical evolution of early time post-detonation event environments did not exist. Our work merged historic data and experimental approaches to support development of a computational framework able to simulate fundamental processes (e.g., entrainment of local environment, oxidation chemistry, and cooling time scales) that may perturb the radionuclide inventory captured in post-detonation debris. Work with historic debris confirmed that entrained environmental material affect debris composition, structure, and radionuclide incorporation. Complementary work utilizing a readily controllable and tunable benchtop setup (a plasma flow reactor) simulated the late cooling of a nuclear fireball (e.g., T < 6000 K) and bounded the sensitivity of actinide speciation and particle size distribution to variations in oxygen concentration and cooling rates. Concurrent laser ablation and laser heating experiments were used to investigate the chemistry and physics of processes occurring in vaporized and/or rapidly heated actinides and other elements in the presence of oxygen. A more computationally efficient microphysical model was developed for predicting and evolving size distributions of particles forming from mixed vapor terms and simulating particle formation processes under a variety of extreme conditions. Continued study of historic nuclear event film confirmed that shockwave data and physics codes agree to within the uncertainty of the data. Good agreement was achieved for thermal emission from an airburst, however the paucity of low-temperature molecular opacity data for mixtures of air, bomb debris, entrained dirt, and water vapor complicate agreement for more elaborate scenarios. A multiphysics code (ALE3D) was modified to bring the necessary physics and chemistry, including these new data and insights, onto a single platform. Code development included improved initialization of large physical systems, modernization of chemistry capabilities, and modifications to enable inclusion of particle transport.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2025

Phonon-Spin Scattering from Unpaired f-electrons in U atoms and It’s Influence on Thermal Transport in Uranium-doped Thorium Dioxide Single Crystals

In this work, impact of low level of uranium (U) atom substitution on thermal conductivity of thorium dioxide (ThO2) is investigated. ThO2 is an electronic insulator with a wide optical band-gap and no unpaired electrons whose thermal transport is governed by phonons. U-substitution introduces unpaired f-electrons resulting in paramagnetic behavior of U-ThO2 at room temperature, which significantly suppresses its thermal conductivity. A single crystal of U-ThO2 with graded composition of U is grown using a hydrothermal synthesis method, and thermal conductivity measurements are performed in regions with uniform composition of U at levels of 0%, 6%, 9% and 16%. Measured thermal conductivity profiles over 77–300 K temperature range are analyzed using an analytical expression for phonon-mediated thermal transport based on Klemens-Callaway model. Temperature dependent thermal conductivity is found to deviate significantly from the Rayleigh scattering trend expected for a simple substitutional point defect with a small perturbation to mass and interatomic forces. With the resonant scattering term, observed large suppression of thermal conductivity at low temperatures can be closely reproduced. Additionally, the extracted phonon-spin coupling constants imply a nonlinear relation of phonon-spin interaction intensity with respect to U doping percentage. Our study reveals how phonon-spin scattering contributed by unpaired f-electrons in U atoms influences thermal transport in the U-ThO2 system.

36 - MATERIALS SCIENCE↗

DOE OSTI2022

System Analysis Modeling and Intermodal Transportation for Commercial Spent Nuclear Fuel

This is a technical presentation that does not take into account contractual limitations or obligations under the Standard Contract for Disposal of Spent Nuclear Fuel and/or High-Level Radioactive Waste (Standard Contract) (10 CFR Part 961). For example, under the provisions of the Standard Contract, spent nuclear fuel in multi-assembly canisters is not an acceptable waste form, absent a mutually agreed to contract amendment.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2026

FY26 Progress Report on the Operation of the Activated Materials Laboratory at the Advanced Photon Source as a Nuclear Science User Facilities Partner Facility

The Activated Materials Laboratory (AML), located in the Long Beamline Building of the Advanced Photon Source (APS) at Argonne National Laboratory (ANL), provides a centralized radiological capability for preparing, handling, and supporting synchrotron experiments on activated materials. As a Nuclear Science User Facilities (NSUF) partner facility, the AML enables the receipt of radioactive shipments, open-form sample handling, encapsulation, transport of specimens to and from APS beamlines, and experimentation with dedicated equipment. The partnership includes the APS 1-ID and 20-ID beamlines, which provide high-energy x-ray scattering, tomography, and diffraction microscopy techniques for ex-situ, in-situ, and grainresolved three-dimensional (3D) characterization. All samples supported through the AML and partner beamlines must meet radiological limits of less than 100 mrem/h at 30 cm. This FY26 progress report summarizes the first full year of AML operations as an NSUF partner facility and highlights progress in both user support and capability development. By the end of FY26, the AML had received a total of 10 NSUF-awarded projects, including 2 Consolidated Innovative Nuclear Research (CINR), 7 Rapid Turnaround Experiment (RTE), and 1 Super RTE projects. Beamtime was fully delivered for 3 RTE projects and partially delivered for 1 CINR project, demonstrating successful workflows for receipt, encapsulation, beamline transfer, and radiological experiment execution. These efforts demonstrated safe radiological experiments at APS beamlines for samples with dose rates above the historical 5 mrem/h threshold and now up to 100 mrem/h at 30 cm, marking an important milestone for neutron-irradiated materials research. During FY26, the AML also expanded its experimental capabilities. A Psylotech xTS load frame with in-grip rotation was deployed for room-temperature mechanical testing with threedimensional x-ray characterization during interrupted loading. A Linkam TS1500V vacuum heater was commissioned for thermally driven studies, and temperature calibration experiments were performed to establish specimen-relevant thermal profiles. In parallel, a customized split-tube furnace for high-temperature mechanical testing entered commissioning, and initial work began on robotic sample handling to reduce worker dose and improve operational efficiency. Data workflow and beamline operations continued to mature. Together, these developments demonstrate that the AML is becoming a unique national resource for safe, efficient, and scientifically advanced characterization of activated materials at the APS.

Zhang, Xuan↗

DOE OSTI2024

Toward a high-fidelity tritium transport modeling for retention and permeation experiments

We report Tritium Migration Analysis Program version 8 (TMAP8), the latest version of TMAP, was developed within the framework of the Multiphysics Object-Oriented Simulation Environment (MOOSE). Created at Idaho National Laboratory (INL), MOOSE is an open-source, dimension-agnostic, fully coupled, and fully implicit multiphysics platform featuring massively parallel computation capabilities. Using TMAP8, tritium transport in a divertor monoblock was analyzed to elucidate the effects of pulsed operation (up to fifty 1,600 s plasma discharge and cool-down cycles) on the tritium in-vessel inventory source term and ex-vessel release term (i.e., tritium retention and permeation) for safety analysis. With its built-in Message Passing Interface capability, TMAP8 can, in under 2 h, simulate tritium transport in three different layered materials (i.e., tungsten, copper, and copper-chromium-zirconium alloy) in 2D geometry, using a single device/computer with 10 cores. The MOOSE-based TMAP8 code can leverage other MOOSE tools developed under the Nuclear Energy Advanced Modeling and Simulation program to perform tritium and thermal transport in complex geometries and multiphysics environments. And via its massively parallel computation, MOOSE will enable the fusion pilot plant designers to conduct high-fidelity multiphysics modeling for the design of the divertor and blanket systems as well as for the safety analysis.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

Effect of supplementary cementitious materials on the degradation of cement-based barriers in radioactive waste repository: A case study in Korea

This study focuses on investigating the chemical degradation characteristics of cementitious barriers used in low- and intermediate-level radioactive waste repository by reactive transport modeling. The impact of the blending with supplementary cementitious materials (SCMs) in the barriers on the chemical degradation was evaluated to find the optimum barrier design. A number of different barrier designs were examined by replacing ordinary Portland cement (OPC) by SCMs (i.e., fly ash, silica fume, and blast-furnace slag). The simulation results showed that silica fume blended barrier has better durability against chemical degradation by rainwater compared to fly ash or blast-furnace slag blended barriers. In addition, the chemical durability of silica fume-based barrier increased with increasing replacement level up to about 20 %. It seems that the amount of formed calcium silicate hydrate (CSH) in the initial cement-based barrier highly affects the overall chemical durability. The newly developed reactive transport model demonstrated its capability for understanding the barrier performance and investigating the optimal design of the barrier system.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2026

Radiation-induced segregation in dilute Fe–Cr: A rate-theory framework for the Cr enrichment–depletion transition at the grain boundary

Radiation-induced segregation (RIS) poses a significant challenge for ferritic Fe–Cr alloys under irradiation, as it can compromise mechanical integrity and increase susceptibility to intergranular corrosion. Yet, the mechanisms governing Cr segregation remain incompletely understood. Here, in this study, we present a physics-based rate-theory model parameterized using self-consistent mean field theory-based Onsager transport coefficients to investigate RIS at the grain boundary in dilute Fe-(0.1 at. %) Cr. Under equal production rates of vacancies and self-interstitial atoms (SIA), and their equal absorption rates by bulk dislocations, the model simulates the experimentally observed transition from Cr enrichment at low temperatures to depletion at higher temperatures. Under these unbiased conditions, systematic investigation reveals that while temperature-dependent transport properties dictate the segregation direction, dose rate, grain size, and dislocation density only influence the magnitude and spatial extent of Cr segregation. However, under more realistic conditions of preferential vacancy production within damage cascade and/or preferential SIA absorption by bulk dislocations, the enrichment-to-depletion transition shifts to lower temperatures. Our findings demonstrate that RIS predictions based solely on transport coefficients are valid only under symmetric point defect flux conditions, and that biases in defect production and absorption must be considered for accurate predictions. This work provides a mechanistic framework for understanding RIS in ferritic alloys and informs alloy design for advanced nuclear systems.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗