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At least 19 records

Angular Correlations of Gamma Rays from Fission Product Solution

Fission products from photon-induced fission are routinely used at Idaho National Laboratory as part of nuclear forensics activities. Typically, the focus is on fission products with relatively large fission yields (Ba-140, Mo-99, etc.). The nuclear data associated with the well-known isotopes have small uncertainties, and many have well-known angular correlations between emitted gamma-rays, if applicable. However, for isotopes with smaller fission yields or less intense gamma-ray emission intensities, the nuclear decay schemes and gamma-ray emission intensities may be less well-known. The Germanium Rotational Measurements for Angular Correlation (GeRMAC) system was designed to use two high-purity germanium (HPGe) detectors in a coincidence counting set-up but allows one of the HPGe detectors to rotate at a constant distance from a radioactive source, changing the relative angle between the two HPGe detectors. Angular correlations can then be determined from the relative photopeak areas between two gamma-rays emitted as part of the same nuclear decay. By recording the HPGe spectra in list mode, the angular correlations of gamma-rays emitted from complex sources, consisting of multiple isotopes, can be measured simultaneously and the individual isotope emissions can be isolated. Using the GeRMAC system, a multi-isotope fission product source, produced with photon-induced fission of U-238, was measured using a single rotational arc (180 degrees) to obtain the angular correlation between gamma-rays emitted by the large number of fission products contained in the solution with an angular accuracy of 1 degree. In particular, La-140 (38 gamma rays) and Nd-147 (26 gamma rays) are of interest to the nuclear forensics community.

46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗

Computer program FPIP-REV calculates fission product inventory for U-235 fission

Computer program calculates fission product inventories and source strengths associated with the operation of U-235 fueled nuclear power reactor. It utilizes a fission-product nuclide library of 254 nuclides, and calculates the time dependent behavior of the fission product nuclides formed by fissioning of U-235.

Brown, W. S.↗

Energy dependence of fission product yields in the second-chance fission region

An extensive dataset of cumulative fission product yields has been generated under a joint collaboration between Los Alamos National Laboratory (LANL), Lawrence Livermore National Laboratory (LLNL), and the Triangle Universities Nuclear Laboratory (TUNL). The energy dependence of the cumulative yield for a select number of high-yield fission products has been measured using quasimonoenergetic neutrons with energies between 5.5 and 11.0 MeV. This is in addition to previously published data covering 0.5–4.5 and 14.8 MeV. The absolute number of fissions was determined during the irradiation period using dual-fission ionization chambers, and the fission products were measured postactivation by whole target γ-ray spectroscopy. Here this paper presents the absolute cumulative fission product yields as a function of incident neutron energy from the neutron-induced fission of 235 U, 238 U, and 239 Pu isotopes at four incident energies in the second-chance fission region and compares them with existing literature values. Corrections relevant to this collaboration's previously published data are also discussed.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Characterization of a platform for the gas transport, collection, and identification of fission products in the high-intensity laser environment

Recent progress in the production of laser accelerated high flux proton beams opens new possibilities for the study of fission in unique environments. To this end, we are currently pursuing the development of a platform for the swift gas transport, collection, and identification of fission products. Fission is induced in targets fixed inside a sealed chamber through which a carrier gas flows, transporting fission products to a carbon filter for collection and online spectroscopy. This has been recently demonstrated using target normal sheath accelerated protons at the PHELIX laser facility. There were large discrepancies between measured rates and those expected based on established fission yields and measured beam parameters. These discrepancies prompted a large number of tests at the Idaho Accelerator Center (IAC), where fission in uranium is induced by bremsstrahlung photons generated by 21 MeV electrons from a linear electron accelerator. Here, the results are compared to a series of models that account for the slowing of energetic fission fragments in the carrier gas and the fluid dynamics of the gas flow that transports fission products to the collection filter. Characterization of the apparatus reveals a few mechanisms that together account for a portion of the previously observed discrepancies at the PHELIX laser facility. However, additional research is necessary before high-accuracy experiments can be performed with the apparatus. Work performed under the auspices of the U.S. Department of Energy by LLNL under contract DE-AC52-07NA27344.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Development and application of sorption mass transfer models for fission product transport in TRISO fuel systems using BISON

Fission product mass transfer within and between TRISO particle and compact layers is an important phenomenon. It directly impacts fission product release predictions, which are used as source terms for safety and licensing calculations. Modeling fission product transport within layers and across bonded interfaces is relatively straightforward under the assumptions of isotropic Fickian diffusion, concentration continuity, and flux continuity. Modeling fission product transport across gaps and debonded layers is more difficult. Gaps are known to form between the buffer and inner PyC (IPyC), and debonding may occur between the IPyC and silicon carbide (SiC). A new mass transfer model was developed to provide a more accurate and robust fission product release calculation by accounting for interlayer sorptivity. One importance of the new model is to account for temperature and material changes across the gap based on sorption isotherm. This work presents the development of the sorption behavioral model and a fission product trapping model, and analyses the subsequent fission product diffusion behavior, specifically cesium, through TRISO particles and compact materials using the BISON fuel performance code.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Fission Product Yield Modeling and Evaluation

Although independent and cumulative fission product yields have been a part of evaluated libraries for decades, there have been few updates over the years. The fission product yield sub-library in the ENDF/B-VIII.0 library is still largely based on the evaluation of England and Rider from the mid-90’s, with only more recent updates to the energy dependence of 239 Pu below 2 MeV and fixes to isomeric states and missing fission products. Over the past several years, there have been a wealth of new measurements of independent and cumulative fission product yields, particularly those with short half-lives, and there have been significant improvements in the modeling of prompt and delayed fission observables. Here, we describe recent progress in the improvement of fission product yield calculations, using the BeoH code and the underlying Hauser Fesh-bach Fission Fragment Decay (HF 3 D) model, developed at Los Alamos National Laboratory. We will describe our recent calculations for consistent prompt and delayed fission observables for major and minor actinides, including new work investigating isomeric ratios. We will detail the ongoing evaluation process for energy-dependent fission product yields from thermal up to 20 MeV incident neutron energy and some validation work that has been performed for these new fission product yield calculations. Additionally, we will discuss future perspectives of this work, highlighting the need for additional data.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

AGR-5/6/7 Irradiation Experiment Fission Product Mass Balance

This report presents the fission product mass balance for the AGR-5/6/7 TRISO fuel irradiation experiment. The fission product inventories deposited on capsule components outside of the fuel (e.g., stainless-steel shells, graphite holders, Grafoil disks, and associated hardware) were quantified as part of the post-irradiation examination (PIE) to assess the performance of this fuel. Comparisons were made between these inventories and depletion calculations, non-destructive measurements of fuel fission product inventories in the intact fuel compacts, prior AGR experiments, and results from among each of the five distinct AGR-5/6/7 capsules. The data served as estimates of the condensable fission products released from the fuel during irradiation. Excluding Capsule 1 (which experienced accidental damage during irradiation) and Capsule 3 (which was tested at very high irradiation temperatures of >1300°C), the results indicate that the AGR-5/6/7 fuel performed comparably to fuel from earlier AGR experiments. The mass balance results were also used to estimate the number of particles with in-pile SiC failures. Subject to the assumptions made in these estimates, and excluding Capsules 1 and 3, the in-pile SiC failure rates for AGR-5/6/7 are comparable to those observed in AGR-2.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

AGR TRISO Fuel Fission Product Release Data Summary

Knowledge of fission product retention in and release from TRISO fuel under normal and off-normal conditions is needed for reactor safety analyses. This is important for coated-particle fuel used in high-temperature reactors relying on the functional containment strategy. Data on the release and retention of key fission products (e.g., Ag-110m, Cs-134, Eu-154, and Sr-90) in AGR UCO TRISO fuels have been summarized in this report, and empirical relationships with respect to time and temperature were developed. This included fission product accumulation in the OPyC and compact graphitic matrix during irradiation, release from compacts during irradiation, and release during post-irradiation safety testing at temperatures from 1600-1800°C. The frequencies of SiC failure and TRISO coating failure from irradiation and post-irradiation safety testing were also summarized as they have bearing on the quantities of Cs release from the fuel. In a forthcoming publication, a framework for combining and using these empirical relationships as part of a source term analysis will be presented.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Energy Dependent Fission Product Yields (2nd year Milestone and Deliverables)

Introduction to the project: One of the Laboratory missions is to provide consistent, high-precision fission product; yield data critical for testing fission models and maintaining the safety and security of the nation’s nuclear weapons stockpile. However, high-quality, energy-differential fission product yield data is missing for certain actinides and neutron energies important to constrain the new U.S. Nuclear Data Program evaluation effort; It has been shown that the reactor antineutrino anomaly may be at least partially caused by roughly 20 fission products. The fission product yield data is missing or incomplete for many of these isotopes, thus it is necessary to accurately determine these values to better constrain the anomaly; Aitor Bracho is measuring very short-lived (seconds to minutes) fission product yields of 235 U and 239 Pu using monoenergetic neutron beams at E n = 60 and 560 keV; Aitor Bracho is using a direct approach utilizing a state-of-the-art rabbit transfer system, superior HPGe detector, and digital acquisition systems for fission decay measurements. The goals of this project: lop experimental capabilities and data analysis techniques to carry out the gamma-ray spectra analysis necessary for fission product yield calculation; Provide high-precision and energy-dependent fission product data supporting fission theory, neutrino physics, and applied physics.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Energy dependence of chain fission product yields from neutron-induced fission of 235 U, 238 U, and 239 Pu

The lack of completeness and systematic studies of cumulative fission product yield (FPY) from the three major actinides of 235 U, 238 U, and 239 Pu, over a broad energy range, was the primary motivation for the LLNL-LANL-TUNL collaboration. Given the focus on resolving FPY behavior around fission spectrum neutron energies, our 2016 data provides FPY measurements in fine energy steps in the range of 0.5–5.5 MeV and an additional anchor point at 14.8 MeV. Recently, our collaboration filled the gap between second chance fission and 14.8 MeV, providing a comprehensive study at eleven incident neutron energies from 0.5 to 14.8 MeV. However, during the course of the last measurements, it was found that the reported masses of the actinide deposits in the fission ionization chambers, which were used to measure the number of fissions, were not consistent with the complementary tests. Therefore, some corrections to the old data are needed. The purpose of this paper is to summarize all of the high-yield FPY data obtained for 235 U, 238 U, and 239 Pu isotopes using quasi-monoenergetic neutron beams at 11 incident energies ranging from E n = 0.5 to 14.8 MeV.

Tonchev, A. P. [Lawrence Livermore National Labora↗

Calculated covariance matrices for fission product yields using BeoH

Fission product yields (FPY) are important for a variety of applications (reactor neutronics, spent fuel, dosimetry, radiochemistry, etc.) and are currently included in many of the evaluated libraries around the world. The FPYs in the current US evaluation, ENDF/B-VIII.0, are mainly based on the 1994 evaluation of England and Rider and have only had slight updates—such as the inclusion of a 2 MeV point for 239 Pu—since their development. Additionally, only mean values and uncertainties are included in the evaluation, not full correlations. Los Alamos National Laboratory, in collaboration with several other institutes, has been working on an updated evaluation for the FPYs of 239 Pu(n,f), 235 U(n,f), 238 U(n,f), and 252 Cf(sf) using the deterministic, Hauser-Feshbach, fission fragment decay code, BeoH. BeoH calculates the FPYs consistently with many other prompt and delayed fission observables, explicitly taking into account multi-chance fission and ensuring consistency between observables. In addition to providing updated means and uncertainties for the FPYs on a pointwise energy grid from thermal to 20 MeV, we calculate correlations between all FPYs at each incident energy and across incident energies. Here, we discuss the development of these covariance matrices, differences in the correlations between FPYs based on the parameters that are included in the model optimization, and correlations across incident energies for neutron-induced fission.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Diffusion behavior of lanthanide fission products in bcc Fe cladding: A first-principles study

Fuel-cladding chemical interaction poses significant challenges in nuclear reactors, where fission products generated from nuclear fuel interact with Fe-based cladding materials, potentially compromising their structural integrity. This study investigates the diffusion behavior of lanthanide fission products, Lanthanum (La), Cerium (Ce), Praseodymium (Pr), and Neodymium (Nd), within body-centered cubic (bcc) Fe cladding using the density functional theory, nudged elastic band method, and self-consistent mean field theory. Our results reveal significant vacancy binding energies, particularly with the 1st and 2nd nearest neighbors, which diminish beyond the 5th nearest neighbor, with La exhibiting the strongest binding affinity, followed by Nd, Ce, and Pr. The nudged elastic band calculations indicate significant high barriers for the dissociation of 1st nearest neighbor vacancy-solute pairs for all fission products. The tracer diffusion coefficients of these fission products were derived in an Arrhenius form, with a magnetic correction that accounts for the high-temperature paramagnetic state. The significant trapping effect of vacancies caused by a very dilute concentration of fission products reduces vacancy mobility, potentially leading to modifications in point defect supersaturation, void nucleation, and swelling under irradiation. These represent critical challenges for irradiated cladding materials. The tracer diffusion coefficients indicate that Nd diffuses the fastest, followed by La, Ce, and Pr. Furthermore, this study provides essential insights for understanding fission product transport in cladding materials and informs future design strategies to mitigate fuel-cladding chemical interaction, ultimately enhancing nuclear reactor safety and performance.

Diffusion↗

Multi-scale fission product release model with comparison to AGR data

TRistructural ISOtropic (TRISO) particle fuel is central to several advanced, high-temperature reactor designs. Each particle consists of a fuel kernel encapsulated by three layers of carbon and ceramics that prevent the release of fission products and ensure physical integrity. Despite outstanding retention properties, fission product release has been observed from intact particles. To better understand and quantify fission product release from TRISO particles, a multiscale, mechanistic model of fission product transport is being developed by the Nuclear Energy Advanced Modeling and Simulation (NEAMS) program. Previous work focused on silver (Ag) transport and improved Ag release predictions. The work described in this report builds on this experience to better understand cesium (Cs) transport in silicon carbide (SiC), the main barrier to the release of fission products. Atomistic simulations provide bulk and grain boundary (GB) Cs diffusivities in SiC, which are used by phase field simulations in the mesoscale code Marmot to determine the temperature, microstructure, and irradiation-dependent Cs diffusivity at the mesoscale in SiC. This approach attributes the different temperature regimes experimentally observed for Cs diffusivities in SiC to a transition from bulk-dominated diffusivity at high temperatures to a GB-dominated regime at low temperatures, providing new insight. The multiscale, mechanistic effective diffusivity is then implemented in the fuel performance code BISON and further validated by comparing Cs release predictions from Advanced Gas Reactor (AGR)-1 and AGR-2 post-irradiation measurements. The new model improves BISON’s predictability. This document also reports improvements made on Ag transport modeling by accounting for different GB types having different diffusivities. Moreover, this report details preliminary efforts to model palladium (Pd) attack of the SiC at the mesoscale using a phase field approach. Pd attack and its impact on accelerated Ag transport remains a misunderstood phenomenon, and we use the model to demonstrate that the formation of lamellae that has been observed in experiments can be explained by the reaction of Pd with SiC to form alternating layers of graphite and Pd 2 Si. This effort aims to improve our understanding of the reaction and eventually provide a model for BISON to account for Pd penetration and its effects on fission product release.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Diffusion Behavior of Oversized Fission Products in bcc Fe Cladding: A First-Principles Study

Fuel-Cladding Chemical Interaction (FCCI) poses significant challenges in nuclear reactors, where fission products from nuclear fuel interact with Fe-based cladding materials, potentially compromising their structural integrity. This study investigates the diffusion behavior of oversized fission products, Pr, Nd, Ce, and La, within bcc Fe cladding using density functional theory (DFT), nudged elastic band (NEB) method, and self-consistent mean field (SCMF) theory. Our results reveal significant long-range vacancy binding energies, particularly up to the 6th nearest neighbor, with La exhibiting the strongest binding affinity, followed by Nd, Ce, and Pr. The NEB calculations indicate significant high barriers for the dissociation of 1nn vacancy-solute pairs for all fission products. The tracer diffusion coefficients of these fission products was derived in Arrhenius form. The significant trapping effect of vacancies by a very dilute amount of fission products reduces vacancy mobility, leading to an oversaturation of point defects, void nucleation, and swelling. These are critical issues for irradiated cladding materials. The tracer diffusion coefficients indicate that Nd diffuses the fastest, followed by La, Ce, and Pr. This study provides essential insights for developing advanced cladding materials and design strategies to mitigate FCCI, ultimately enhancing nuclear reactor safety and performance.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Rapid separation of radiopure yttrium-91 for tracer studies from mixed fission products and uranium

A novel, single step method for isolating 91 Y from irradiated uranium and mixed fission products has been developed based on the commercially available Eichrom LN resin. The separation procedure allows for loading an LN resin column with an irradiated uranium solution, containing mixed fission products, in dilute HCl where both uranium and yttrium are retained on the resin. Eluting dilute (0.5–1 M) HCl will strip the majority of fission products. Furthermore, increasing the concentration to 3 M HCl will elute 91 Y without the presence of any other fission products. Finally, uranium can be recovered by passing concentrated HCl through the column.

Chromatography↗

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↗

PARFUME/BISON Fission Product Release Predictions versus AGR-3/4 Heating Test Measurements

The fuel performance modeling codes PARFUME (PARticle FUel ModEl) and BISON were used to predict the release of fission products silver, cesium, and strontium from as-irradiated fuel compacts containing tristructural isotropic (TRISO) coated particles during heating tests post irradiation. The AGR-3/4 fuel compacts were irradiated as part of the third and fourth series of planned experiments to support the Advanced Gas Reactor (AGR) program. The heating tests were conducted at temperatures between 1200°C and 1700°C to simulate reactor accident conditions. The measured fission product release fractions from the heating tests were compared to modeling predictions calculated by PARFUME and BISON to evaluate how the codes compare to experimental results. Comparisons between the experimental measured fission product release fractions from silver, cesium and strontium indicate that both modeling codes overpredict the fission product release fractions demonstrating that the diffusivities used in the codes are overestimated. This results in a conservative estimate predicted by the codes when evaluating the fission product release relative to experimental data as it pertains to silver, cesium, and strontium.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗