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DOE OSTI2022

Energy Dependent Fission Product Yields

Since 2011, the LLNL-LANL-TUNL collaboration has undertaken experimental measurements of the energy evolution of the chain fission product yields (FPY) from neutron-induced fission of 235 U, 238 U, and 239 Pu using quasi-monoenergetic neutrons produced at the TUNL 10 MV Van de Graaff accelerator. Our method relies on direct, post-irradiation γ-ray spectroscopy of γ-rays emitted by fission products in actinide targets, with multiple γ-ray spectra taken continuously for a period from a half-hour to three months from the end of irradiation. The main experimental results of this study have been published for eight incident neutron energies of En = 0.58, 1.37, 2.37, 3.6, 4.6, 5.5, 8.9 and 14.8 MeV [1–4]. For each incident energy, approximately 16 cumulative FPYs were determined, nearly all being high-yield fission products, i.e., those occurring in the peaks of the mass distributions. As will be described in this report, our FPY analysis has been significantly improved in every step of the process, reducing the overall systematic uncertainties compared to previously published data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

Standardizing a Renewed Fission Product Yield Library and Related Covariances (Part II)

A complete library of independent fission product yields including covariance information was generated by a sequential Bayesian methodology whose prior information consisted of independent fission product yields and branching ratios of the possible decay modes reported in the recently released ENDF/B-VIII.0 nuclear data library. The Bayesian procedure consisted in the adjustment of independent fission product yields to match the set of stable and long-lived cumulative yields reported in the ENDF/B-VIII.0 nuclear data library which, in this work, were considered as legacy values together with their uncertainties. According to the χ 2 -metric, the results obtained by this methodology show a systematic improvement in the agreement with legacy reported cumulative yields for the entire adjusted independent fission product yield library.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Earth Filter Mathematica Toolbox V4 User’s Guide: Simplifying, Visualizing and Quick Modeling of All Fission Products from 60 Nuclear Sources

The Earth Filter Mathematica toolbox is a set of user-friendly routines that accurately calculate the ingrowth and decay of any of the 908 fission products for an infinite combination of sources over a large dynamic range and large time scales. This toolbox was developed by Dr. W. P. Brug at Los Alamos National Laboratory and eliminates the need for the user to define and solve differential equations by automatically scanning the ENDF-349 dataset and creating a complete set of differential equations (including delayed neutron branches to both the ground and metastable states) for every fission product. Additionally, this code allows the user to choose the data source for half-lives from several key references (i.e., TORI, IAEA, ENDF or NUDAT.) The complete set of ENDF-349 independent and cumulative fission yields for all 60 isotopic targets and 4 different neutron spectrums are included. This allows nearly any nuclear fission source to be accurately modeled as a linear combination of endpoint sources. The Earth Filter Toolbox has no limit as to the length of split list, and split lists of 5 or more endpoint sources can be quite common.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

Fission with Exotic Nuclei (Full Technical Report)

Despite its importance for stockpile stewardship or nuclear forensics, data on fission is fragmentary: most experiments have only been performed on stable actinide nuclei and are often incomplete, and theoretical simulations often contain many parameters hard to constrain, which results in large uncertainties. Consequently, nuclear libraries have large gaps for important isotopes. The goal of this project was to prepare to take advantage of the unprecedented yields of radioactive isotopes at the upcoming DOE Facility for Rare Ion Beams and to leverage recent progress in the field of machine learning to develop a comprehensive program of fission studies that could address some of the most pressing problems in nuclear fission over the next several decades. Our project leveraged synergies between experimental nuclear physics, nuclear theory, and data science expertise at LLNL. On the experimental front, our main objective was to develop in-house expertise for inverse kinematics reactions with relativistic beams as well as to field and test new detectors to perform correlated measurements of fission properties. On the theoretical side, the objective was to develop a novel, high-fidelity and scalable approach of fissionfragment calculations based on emulating computationally expensive, quantum-mechanical calculations of nuclear properties with deep neural networks.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

Measurement of the Neutron-Induced Capture-to-Fission Cross Section Ratio in 233 U at LANSCE [Slides]

This presentation finds that new measurement at LANSCE combining DANCE and NEUANCE at the end of 2020 and 2021. Additionally, two samples of 10 mg and 20 mg of 233 U have been prepared at LANL by Evelyn M. Bond (December 2020). Data analysis has been finished and results of the capture-to-fission ratio on 233 U in the neutron energy region from 0.7 eV to 250 keV have been provided. The focus was to provide data from 1-300 keV. We are providing data from 0.7 eV to 1 keV in addition. The result has been normalized to the ENDF/B-VIII.0 broadened capture-to-fission cross section ratio in the neutron energy region recommended by the Luiz Leal and Marco Pigni, between 8.1 and 14.7 eV. This is the first measurement of the capture-to-fission ratio between 2 - 30 keV. The data show some small differences in the RRR with the evaluation though the general trend is consistent. In the URR this data shows a smaller capture-to-fission ratio than the evaluation from 10 to 150 keV

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Development of bubble evolution model for new mechanistic transient fission gas release capability in BISON

This report summarizes efforts within NEAMS to investigate the mechanisms that govern fission gas behavior in UO 2 . In particular, the focus is on understanding how fission gas behavior causes transient fission gas release and fragmentation/pulverization of high burnup structure (HBS) in UO 2 . HBS forms in the periphery of the pellet where temperatures are relatively low. Previously, MD simulations were performed to determine the reaction energies for various Xe and U defects with bubbles, as a function of Xe to vacancy ratio or, equivalently, pressure. As had been shown in FY22, it was found that the unmodified version of the Simple Integrated Fission Gas Release and Swelling (SIFGRS) model within BISON greatly over-predicted the number gas atoms per vacancy in the bubbles in the outer rim of the pellet (a ratio of > 1 million). This was due to slow grain boundary vacancy diffusivity and not accounting for the pressure-dependent reaction energy for Xe interstitials with bubbles. The application of the pressure dependent reaction energies was able to restrict Xe to vacancy ratios to 2:1, which is far more realistic than those originally obtained from SIFGRS.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Lower-length-scale modeling of chemical additions, corrosion and fission products in select MSR base salts

Molten salts play a crucial role in advancing Generation IV nuclear energy technology, with chloride-based salts like NaCl-UCl 3 garnering significant attention due to their distinctive properties. However, the corrosive nature of molten salts causes the dissolution of chromium (Cr), leading to the formation of CrCl 2 and CrCl 3 species in molten chlorides. Moreover, the radioactive decay of nuclear fuel gives rise to fission products, including Cs, Sr, and I chlorides. The first part of this report presents a comprehensive study utilizing ab initio molecular dynamics (AIMD) simulations to investigate the properties of eutectic NaCl-UCl 3 molten salt in the presence of corrosion products (CrCl 2 and CrCl 3 ) and fission product (CsCl). The study focuses on essential structural and thermophysical properties such as density, mixing energy, coordination numbers (CN), and Radial Distribution Functions (RDF) of the salts with varying compositions of corrosion products and fission product, covering a range from 0% to 13.5%. The results offer valuable insights into the behavior of corrosion and fission products in uranium-based molten salts, providing essential data that can be used as input to the MTDB-TC and MSTDB-TP property databases being developed by the NEAMS program. Due to their favorable characteristics such as low melting points, high boiling points, and low costs, MgCl 2 +NaCl+KCl (MNK) eutectic salts have recently attracted attention as high-temperature heat transfer fluids. The incorporation of LiCl into MNK salts can further reduce their melting points and increase their specific heat capacities, which is de- sirable for high-temperature heat transfer applications. The second part of this report presents the development and validation of a new shell-model potential for the MgCl 2 +NaCl+KCl+LiCl system, which captures the polarization of Cl anions. The extensive comparison with experimental data and AIMD simulations demonstrates the accuracy and reliability of the potential. Furthermore, using this potential, we elucidate the intricate network structure in MNK eutectic salts that is formed through polyhedron sharing. This research contributes to a fundamental understanding of the atomic structures and thermophysical properties of multi-component molten salts, which is crucial for future development of heat transfer fluids for applications in molten salt reactors.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Behavior of contaminants and simulant fission products in the advanced chlorination process

The University of Tennessee, Knoxville and Oak Ridge National Laboratory have completed proof-of principle testing on an advanced sulfur-based zirconium and aluminum chlorination process for the recovery of Zr or Al from spent fuel claddings and purification of the products. This process could be used to recover hafnium-free nuclear-grade zirconium for reuse or disposal as low-level waste. Testing showed that even non-optimized reaction protocols could produce zirconium product streams from simulated irradiated fuel with purities >90%. The chlorination process was tested on representative fission product species that would be found in Advanced Test Reactor fuel (ATR). First, fission product generation was determined through modeling and simulation of the ATR. The generation of fission products was used to selected contaminants and potentially volatile fission product simulants for laboratory testing. The goal is to identify which species may react with the sulfur-chlorine reagents and be transported into the advanced chlorination off-gas.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Coproduction of Light and Heavy r-process Elements via Fission Deposition

We apply for the first time fission yields determined across the chart of nuclides from the macroscopic-microscopic theory of the Finite Range Liquid Drop Model to simulations of rapid neutron capture (r-process) nucleosynthesis. With the fission rates and yields derived within the same theoretical framework utilized for other relevant nuclear data, our results represent an important step toward self-consistent applications of macroscopic-microscopic models in r-process calculations. The yields from this model are wide for nuclei with extreme neutron excess. We show that these wide distributions of neutron-rich nuclei, and particularly the asymmetric yields for key species that fission at late times in the r process, can contribute significantly to the abundances of the lighter heavy elements, specifically the light precious metals palladium and silver. Since these asymmetric yields correspondingly also deposit into the lanthanide region, we consider the possible evidence for coproduction by comparing our nucleosynthesis results directly with the trends in the elemental ratios of metal-poor stars rich in r-process material. We show that for r-process enhanced stars palladium over europium and silver over europium display mostly flat trends suggestive of coproduction and compare to the lanthanum over europium trend which is often used to justify robustness arguments in the lanthanide region. We find that such robustness arguments may be extendable down to palladium and heavier and demonstrate that fission deposition is a mechanism by which such a universality or robustness can be achieved.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Ignition of Carbon Burning from Nuclear Fission in Compact Stars

Abstract Type Ia supernovae (SN Ia) are powerful stellar explosions that provide important distance indicators in cosmology. Recently, we proposed a new SN Ia mechanism that involves a nuclear fission chain reaction in an isolated white dwarf (WD). The first solids that form as a WD starts to freeze are actinide rich and potentially support a fission chain reaction. In this Letter, we explore thermonuclear ignition from fission heating. We perform thermal diffusion simulations and find at high densities, above about 7 × 10 8 g cm −3 , that fission heating can ignite carbon burning. This could produce an SN Ia or another kind of astrophysical transient.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS1978

Power deposition in volumetric /U-235/F6-He fission-pumped nuclear lasers

The power deposition in (U-235)F6-He fission-pumped nuclear lasers is studied. Specifically, means to maximize the energy density in the He gas are assessed. Primary loss mechanisms are identified as the fission-fragment transport to the laser-cell wall and UF6 gas excitation. The losses are thus strongly dependent on UF6 concentration. It is found that maximum power will be deposited in a laser tube when the tube radius is as large as the range of fission fragments. Experimental results indicate that when the tube radius equals the fission-fragment range, the ratio of a UF6 partial pressure to total pressure is 0.15, and the UF6-He mixing ratio is 1:6, maximum power will be deposited.

Wilson, J. W.↗

NASA NTRS1982

Fission track studies of xenolithic chondrites - Implications regarding brecciation and metamorphism

Fission tracks in phosphates from one gas-poor chondrite and three gas-rich ones are studied to determine their thermal history and brecciation time scales. Model fission track ages are calculated for given track densities due to Pu-244 and U-238; track densities and uranium measurements for whitlockite are shown, and possible sources of the tracks are mentioned. Details of track density and uranium measurements are discussed for each meteorite separately. Whitlockites from all the meteorites give model fission track ages of 4.4 Gyr assuming a Pu/U ratio at 4.55 Gyr of 0.045. The final brecciation event definitely did not reset the track clock in phosphates of one meteor and probably not in another two. It is concluded that the observed fission track ages date the end of metamorphic cooling in the meteorite parent bodies and support the planetesimal model for the formation of xenolithic chondrites.

Kothari, B. K.↗

NASA NTRS1999

Simulated Atomic Fission Engine (S.A.F.E)

This paper presents viewgraphs of S.A.F.E. (Simulated Atomic Fission Engine). The topics include: 1) Why Space Fission Propulsion? 2) History of Fission System Development; 3) New Approach to Space Fission Propulsion System Development; 4) Propulsion Flight Demonstrator Schematic Flight Configuration; 5) Ongoing Propellant Energy Source Tests; 6) First Generation Propulsion System Status; 7) Tungsten Fuel Pin Simulator Tests; 8) Full Module Test (High Efficiency Mode); and 9) First Generation Propulsion Flight Demonstrator Status.

VanDyke, Melissa↗

NASA NTRS2006

Fission Surface Power for the Exploration and Colonization of Mars

The colonization of Mars will require abundant energy. One potential energy source is nuclear fission. Terrestrial fission systems are highly developed and have the demonstrated ability to safely produce tremendous amounts of energy. In space, fission systems not only have the potential to safely generate tremendous amounts of energy, but could also potentially be used on missions where alternatives are not practical. Programmatic risks such as cost and schedule are potential concerns with fission surface power (FSP) systems. To be mission enabling, FSP systems must be affordable and programmatic risk must be kept acceptably low to avoid jeopardizing exploration efforts that may rely on FSP. Initial FSP systems on Mars could be "workhorse" units sized to enable the establishment of a Mars base and the early growth of a colony. These systems could be nearly identical to FSP systems used on the moon. The systems could be designed to be safe, reliable, and have low development and recurring costs. Systems could also be designed to fit on relatively small landers. One potential option for an early Mars FSP system would be a 100 kWt class, NaK cooled system analogous to space reactors developed and flown under the U.S. "SNAP" program or those developed and flown by the former Soviet Union ("BUK" reactor). The systems could use highly developed fuel and materials. Water and Martian soil could be used to provide shielding. A modern, high-efficiency power conversion subsystem could be used to reduce required reactor thermal power. This, in turn, would reduce fuel burnup and radiation damage .effects by reducing "nuclear" fuels and materials development costs. A realistic, non-nuclear heated and fully integrated technology demonstration unit (TDU) could be used to reduce cost and programmatic uncertainties prior to initiating a flight program.

Houts, Mike↗

NASA NTRS2007

Testing in Support of Fission Surface Power System Qualification

The strategy for qualifying a FSP system could have a significant programmatic impact. The US has not qualified a space fission power system since launch of the SNAP-10A in 1965. This paper explores cost-effective options for obtaining data that would be needed for flight qualification of a fission system. Qualification data could be obtained from both nuclear and non-nuclear testing. The ability to perform highly realistic nonnuclear testing has advanced significantly throughout the past four decades. Instrumented thermal simulators were developed during the 1970s and 1980s to assist in the development, operation, and assessment of terrestrial fission systems. Instrumented thermal simulators optimized for assisting in the development, operation, and assessment of modern FSP systems have been under development (and utilized) since 1998. These thermal simulators enable heat from fission to be closely mimicked (axial power profile, radial power profile, temperature, heat flux, etc.) and extensive data to be taken from the core region. For transient testing, pin power during a transient is calculated based on the reactivity feedback that would occur given measured values of test article temperature and/or dimensional changes. The reactivity feedback coefficients needed for the test are either calculated or measured using cold/warm zero-power criticals. In this way non-nuclear testing can be used to provide very realistic information related to nuclear operation. Non-nuclear testing can be used at all levels, including component, subsystem, and integrated system testing. FSP fuels and materials are typically chosen to ensure very high confidence in operation at design burnups, fluences, and temperatures. However, facilities exist (e.g. ATR, HFIR) for affordably performing in-pile fuel and materials irradiations, if such testing is desired. Ex-core materials and components (such as alternator materials, control drum drives, etc.) could be irradiated in university or DOE reactors to ensure adequate radiation resistance. Facilities also exist for performing warm and cold zero-power criticals.

Houts, Mike↗

NASA NTRS2008

A Review of Radiolysis Concerns for Water Shielding in Fission Surface Power Applications

This paper presents an overview of radiolysis concerns with regard to water shields for fission surface power. A review of the radiolysis process is presented and key parameters and trends are identified. From this understanding of the radiolytic decomposition of water, shield pressurization and corrosion are identified as the primary concerns. Existing experimental and modeling data addressing concerns are summarized. It was found that radiolysis of pure water in a closed volume results in minimal, if any net decomposition, and therefore reduces the potential for shield pressurization and corrosion. With the space program focus m emphasize more on permanent return to the Moon and eventually manned exploration of Mars, there has been a renewed look at fission power to meet the difficult technical & design challenges associated with this effort. This is due to the ability of fission power to provide a power rich environment that is insensitive to solar intensity and related aspects such as duration of night, dusty environments, and distance from the sun, etc. One critical aspect in the utilization of fission power for these applications of manned exploration is shielding. Although not typically considered for space applications, water shields have been identified as one potential option due to benefits in mass savings and reduced development cost and technical risk (Poston, 2006). However, the water shield option requires demonstration of its ability to meet key technical challenges including such things as adequate natural circulation for thermal management and capability for operational periods up to 8 years. Thermal management concerns have begun to be addressed and are not expected to be a problem (Pearson, 2007). One significant concern remaining is the ability to maintain the shield integrity through its operational lifetime. Shield integrity could be compromised through shield pressurization and corrosion resulting from the radiolytic decomposition of water.

Schoenfeld, Michael P.↗

NASA NTRS2008

Development and Utilization of Space Fission Power Systems

Space fission power systems could enable advanced civilian space missions. Terrestrially, thousands of fission systems have been operated since 1942. In addition, the US flew a space fission system in 1965, and the former Soviet Union flew 33 such systems prior to the end of the Cold War. Modern design and development practices, coupled with 65 years of experience with terrestrial reactors, could enable the affordable development of space fission power systems for near-term planetary surface applications.

Houts, Michael↗

NASA NTRS2009

Development and Utilization of Space Fission Power Systems

Houts, Michael G.↗