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DOE OSTI2019

Improved Cumulative Fission Yield Measurements with Fission Spectrum Neutrons on 235 U

Two isotopically-characterized targets of high-purity (99.84±0.03%) 235 U-oxide and a neutron dosimetry package were exposed to a pulsed neutron irradiation using the Godiva critical assembly at the National Criticality Experiments Research Center. Following irradiation, the fissioned targets were counted with a broad-energy germanium detector. Estimates of the total fissions for each target were made using measurements of well-known fission products. The total fission values were then used to measure the fission yields of 21 fission products with half-lives between 636 and 119,700 seconds. Mean values of seventeen of the measured fission products fell within the 95% confidence level of the Evaluated Nuclear Data Files VII.1/b (ENDF/B-VII.1) using the larger of the two uncertainties: 84g Br, 89 Rb, 91 Sr, 93 Y, 97 Zr, 101 Mo, 105 Ru, 128 Sn, 129 Sb, 130g Sb, 131 Sb, 131m Te, 133 I, 135 I, 141 Ba, 142 Ba, and 142 La. Seven isotopes were measured to better precision than is listed in the ENDF/B-VII.1 database: 89 Rb, 93 Y, 128 Sn, 129 Sb, 130g Sb, 131m Te, and 133 I. Four of the measured isotopes were found to be statistically different from the ENDF/B-VII.1 database: 94 Y, 134 Te, 134 I, and 138 Xe. Two of the isotopic analyses conducted in this paper fit the parent and daughter data simultaneously. The parent-daughter pairs measured in this way were the 134 Te/I and 142 Ba/La pairs. The fission yield results obtained in this way are unique, especially for 134 I, because the parent and daughter half-lives are so close. Here, given the limited number of direct measurements of the 134 Te/I pair from fast neutron induced fission and the seemingly high estimate for 134 Te from previous work, it is likely that the value in this paper is more accurate; however, additional measurements of this pair are needed to validate this assertion.

42 ENGINEERING↗

DOE OSTI2020

Improved Cumulative Fission Yield Measurements with Fission Spectrum Neutrons on 238U

Two isotopically-characterized targets of high-purity (99.961±0.002%) 238U metal and a neutron dosimetry package were exposed to a pulsed neutron irradiation using the Godiva IV critical assembly at the National Criticality Experiments Research Center to measure the integral fission product yields produced in a Watt fission neutron-energy spectrum. Following irradiation, the fissioned targets were counted with two broad energy germanium detectors. Estimates of the total fissions for each target were made using measurements of well-known fission products. The total number of fissions in each target were then used to measure the fission yields of 33 fission products, 18 of which are published as new measurements. Twelve of the 18 isotopes were in agreement with ENDF/B- VIII.0 using the zeta test and treating ENDF/B-VIII.0 as the true mean: 84mBr, 93Y, 94Y, 104Tc, 134I, 135I, 138Xe, 141Ba, 142Ba, 142La, 146Ce, and 149Nd. The ENDF/B-VIII.0 fission yield for 139Ba was only slightly outside of 1-s relative to the uncertainty measured in this work. Uncertainties for 5 fission product yields were markedly improved over those reported in ENDF/B-VIII.0: 128Sn, 129Sb, 130gSb, 131mTe, and 133I. The fission yields measured for 128Sn, 131mTe, and 133I were in good agreement with the ENDF/B-VIII.0 predicted fission yields. However, fission yields measurements of the isotopes 129Sb, and 130gSb deviated from the ENDF/B-VIII.0 value. Both of these isotopes reside near the doubly magic nuclear shell closures of 50 protons and 82 neutrons. These fission yields may be suppressed because of the odd-odd nuclear structure of 130gSb and the odd-even structure of 129Sb and isomer splitting. Comparisons to other recent work and a brief review with citations are included to support this conclusion.

Fission Yields↗

DOE OSTI2021

Compilation and Evaluation of Isomeric Fission Yield Ratios

Fission yields are essential data for reactor physics, forensics, and astrophysics. In some cases, the fission yield of a fragment is divided between the ground state and a long-lived excited state, and the relative population of the two states is referred to as the isomeric ratio. In this work, we present a comprehensive compilation of experimental isomeric fission yield ratios for all target and projectile combinations. When possible, these data are combined to provide recommended isomeric fission yield ratios for low energy neutron-induced fission and spontaneous fission. The recommended ratios are compared to the traditional Madland-England model, which attempts to describe the isomeric ratios with a single parameter relating to the angular momentum of the fragment. It is found that the model does not reliably reproduce isomeric ratios outside the few nuclei it was fitted to, and its simplified treatment of the statistical process following population in fission results in average spin values, which are neither constant nor follow a recently observed saw-tooth pattern.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2025

Reviewing Incident Neutron Energy assignments in 238 U(n,f) Fission Yield Data

Fission yield evaluations rely not only on precise measurements, but also on clear documentation of experimental conditions especially the energy of incident neutrons inducing fission. In the EXFOR database, following the convention adopted in past evaluations, the incident neutron energy has traditionally been divided in only three energy groups: thermal, fast and 14 MeV. The information is stored in the EN-DUMMY field, which often serves as a placeholder in the presence of broad-spectrum or reactor-based sources. This work reviews 238 U(n,f) entries in EXFOR that use EN-DUMMY, identifying cases where better energy estimates can be made based on the original publications, facility characteristics, or reconstructed neutron spectra. We assign new cross-section-weighted average energies where possible. The revised independent and cumulative fission yield data are compiled for future use in model development and evaluation efforts.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2023

Cumulative fission yields of short-lived fission products from 235 U and 239 Pu measured by HPGe gamma-ray spectroscopy

In this study, we present a preliminary investigation focused on determining cumulative fission yields for short-lived fission products. Our analysis involves examining gamma spectra from the irradiated samples of 235 U and 239 Pu using the High Flux Isotope Reactor. The motivation stems from the observed discrepancy in the antineutrino energy spectrum within the range of 5 to 7 MeV. While several hypotheses have been proposed, a thorough analysis of fission yields provides an additional way of gaining insight into this unexplained phenomenon. Our study suggests that the measured gamma rays from 100 Nb, 140 Cs and 95 Sr are consistent with the expected values. However, 93 Rb, 96 Y, 97 Y and 142 Cs cannot be quantified due to insufficient statistics, interference from other gamma rays and the Compton scattering background. Additionally, the calculated cumulative fission yields based on the measured 140 Cs and 95 Sr are found to be consistent with the JEFF3.3 fission yield library. In conclusion, the present work shows that the potential of improving gamma-ray spectroscopy in the fission yields as a means to improve our understanding of the antineutrino spectrum.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

Stochastically estimated covariance matrices for independent and cumulative fission yields in the ENDF/B-VIII.0 and JEFF-3.3 evaluations

A Monte-Carlo method for the generation of correlation and covariance matrices for independent and cumulative fission yields has been developed. The method uses a constrained Monte-Carlo resampling structure in order to vary evaluated fission yield libraries in a way that meets basic conservation principles. This results in the generation of correlation/covariance matrices with limited model bias and uncertainty; the matrices are primarily reflective of the evaluated fission yield uncertainties and correlations that arise from the evaluation process. This method has been applied to generate correlation and covariance matrices for all of the fissioning systems of the ENDF/B-VIII.0 and JEFF-3.3 evaluations, marking the first time such matrices have been generated for all of these systems. These covariance matrices have been published online for immediate public use. These correlation and covariance matrices can be used to improve uncertainty estimation in calculations of reactor antineutrino emission rates, decay heat problems, and nuclear forensics.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2019

Using excitation-energy dependent fission yields to identify key fissioning nuclei in r -process nucleosynthesis

The possibility that nucleosynthesis in neutron star mergers may reach fissioning nuclei introduces significant uncertainties in predicting the relative abundances of $r$-process material from such events. We evaluate the impact of using sets of fission yields given by the 2016 GEF code for spontaneous (sf), neutron-induced $((n, f))$, and $β$-delayed (βdf) fission processes which take into account the approximate initial excitation energy of the fissioning compound nucleus. We further explore energy-dependent fission dynamics in the $r$ process by considering the sensitivity of our results to the treatment of the energy sharing and de-excitation of the fission fragments using the FREYA code. We show that the asymmetric-to-symmetric yield trends predicted by GEF 2016 can reproduce the high-mass edge of the second $r$-process peak seen in solar data and examine the sensitivity of this result to the mass model and astrophysical conditions applied. We consider the effect of fission yields and barrier heights on the nuclear heating rates used to predict kilonova light curves. We find that fission barriers influence the contribution of 254 Cf spontaneous fission to the heating at ~100 d, such that a light curve observation consistent with such late-time heating would both confirm that actinides were produced in the event and imply the fission barriers are relatively high along the 254 Cf β-feeding path. We lastly determine the key nuclei responsible for setting the r-process abundance pattern by averaging over thirty trajectories from a 1.2–1.4 M ⊙ neutron star merger simulation. Finally, we show it is largely the odd-N nuclei undergoing $(Z, N)(n, f)$ and $(Z, N)β$df that control the relative abundances near the second peak. We find the 'hot spots' for β-delayed and neutron-induced fission given all mass models considered and show most of these nuclei lie between the predicted $N$ = 184 shell closure and the location of currently available experimental decay data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2016

Development of a “Fission-proxy” Method for the Measurement of 14-MeV Neutron Fission Yields at CAMS

Relative fission yield measurements were made for 50 fission products from 25.6±0.5 MeV alpha-induced fission of Th-232. Quantitative comparison of these experimentally measured fission yields with the evaluated fission yields from 14-MeV neutron-induced fission of U-235 demonstrates the feasibility of the proposed fission-proxy method. This new technique, based on the Bohr-independence hypothesis, permits the measurement of fission yields from an alternate reaction pathway (Th-232 + 25.6 MeV α → U-236* vs. U-235 + 14-MeV n → U-236*) given that the fission process associated with the same compound nucleus is independent of its formation. Other suitable systems that can potentially be investigated in this manner include (but are not limited to) Pu-239 and U-237.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

DOE OSTI2018

Development of a “fission-proxy” method for the measurement of 14-MeV neutron fission yields

Here, telative fission-yield measurements were made for 50 fission products from 25.6±0.5 MeV α -induced fission of Th-232. Quantitative comparison of these experimentally measured yields with the evaluated fission yields from 14-MeV neutrons on U-235 demonstrates the application of the Bohr-independence hypothesis for measuring fission yields. As optimum particle-target configurations may be impossible or compromised at a given facility, this new approach, fission-proxy, allows the measurement of fission yields for a given compound nucleus from an alternate reaction pathway since formation and subsequent decay are independent processes.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2016

Effects of fission yield data in the calculation of antineutrino spectra for U 235 ( n , fission ) at thermal and fast neutron energies

Fission yields form an integral part of the prediction of antineutrino spectra generated by nuclear reactors, but little attention has been paid to the quality and reliability of the data used in current calculations. Following a critical review of the thermal and fast ENDF/B-VII.1 235 U fission yields, deficiencies are identified and improved yields are obtained, based on corrections of erroneous yields, consistency between decay and fission yield data, and updated isomeric ratios. These corrected yields are used to calculate antineutrino spectra using the summation method. An anomalous value for the thermal fission yield of 86 Ge generates an excess of antineutrinos at 5–7 MeV, a feature which is no longer present when the corrected yields are used. Thermal spectra calculated with two distinct fission yield libraries (corrected ENDF/B and JEFF) differ by up to 6% in the 0–7 MeV energy window, allowing for a basic estimate of the uncertainty involved in the fission yield component of summation calculations. Lastly, the fast neutron antineutrino spectrum is calculated, which at the moment can only be obtained with the summation method and may be relevant for short baseline reactor experiments using highly enriched uranium fuel.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2015

Fission yield calculation using toy model based on Monte Carlo simulation

Toy model is a new approximation in predicting fission yield distribution. Toy model assumes nucleus as an elastic toy consist of marbles. The number of marbles represents the number of nucleons, A. This toy nucleus is able to imitate the real nucleus properties. In this research, the toy nucleons are only influenced by central force. A heavy toy nucleus induced by a toy nucleon will be split into two fragments. These two fission fragments are called fission yield. In this research, energy entanglement is neglected. Fission process in toy model is illustrated by two Gaussian curves intersecting each other. There are five Gaussian parameters used in this research. They are scission point of the two curves (R{sub c}), mean of left curve (μ{sub L}) and mean of right curve (μ{sub R}), deviation of left curve (σ{sub L}) and deviation of right curve (σ{sub R}). The fission yields distribution is analyses based on Monte Carlo simulation. The result shows that variation in σ or µ can significanly move the average frequency of asymmetry fission yields. This also varies the range of fission yields distribution probability. In addition, variation in iteration coefficient only change the frequency of fission yields. Monte Carlo simulation for fission yield calculation using toy model successfully indicates the same tendency with experiment results, where average of light fission yield is in the range of 90<A<100 and average of heavy fission yield is in about 135<A<145.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2015

Testing actinide fission yield treatment in CINDER90 for use in MCNP6 burnup calculations

Most of the development of the MCNPX/6 burnup capability focused on features that were applied to the Boltzman transport or used to prepare coefficients for use in CINDER90, with little change to CINDER90 or the CINDER90 data. Though a scheme exists for best solving the coupled Boltzman and Bateman equations, the most significant approximation is that the employed nuclear data are correct and complete. Thus, the CINDER90 library file contains 60 different actinide fission yields encompassing 36 fissionable actinides (thermal, fast, high energy and spontaneous fission). Fission reaction data exists for more than 60 actinides and as a result, fission yield data must be approximated for actinides that do not possess fission yield information. Several types of approximations are used for estimating fission yields for actinides which do not possess explicit fission yield data. The objective of this study is to test whether or not certain approximations of fission yield selection have any impact on predictability of major actinides and fission products. Further we assess which other fission products, available in MCNP6 Tier 3, result in the largest difference in production. Because the CINDER90 library file is in ASCII format and therefore easily amendable, we assess reasons for choosing, as well as compare actinide and major fission product prediction for the H. B. Robinson benchmark for, three separate fission yield selection methods: (1) the current CINDER90 library file method (Base); (2) the element method (Element); and (3) the isobar method (Isobar). Results show that the three methods tested result in similar prediction of major actinides, Tc-99 and Cs-137; however, certain fission products resulted in significantly different production depending on the method of choice.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Update of the Cesium-136 Cumulative Fission Yields at Multiple Neutron Energies

Nuclear data is foundational to several fields, including nuclear forensics. Nuclear forensics investigations of fission events, relies heavily on the cumulative fission yields, however several highly useful fission products suffer from very poor nuclear data including cumulative fission yields or associated uncertainties in that value. Cesium-136 is a highly relevant example of this issue, where the cumulative fission yield may be accurate but its uncertainty high enough to preclude its usefulness. In this work we evaluate and calculate an updated cumulative fission yield for 136 Cs for 235 U, 238 U, and 239 Pu at multiple neutron energies or sources using data obtained from irradiation campaigns. In all cases these newly determined cumulative fission yields provided small changes to the actual fission yields but had dramatic improvements to the uncertainty in those yields. These improvements in uncertainty will enable nuclear forensics end users to use 136 Cs data with more confidence.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

Summary Report of the 1st RCM of the CRP on the Updating Fission Yield Data for Applications

The First Research Coordination Meeting of the CRP on “Updating Fission Yield Data for Applications” was held by video conference from 31 August to 4 September 2020 with more than 50 international experts from 16 countries attending the meeting. The CRP is devoted to evaluation efforts of cumulative and independent fission yields for incident energies from the thermal point up to 14 MeV on actinide targets. Produced fission yield evaluations should include full uncertainty quantification and are expected to combine available experimental data and state-of-art model information. Four working groups were created within the collaboration: 1) Availability of experimental fission product yield data for evaluations; 2) New fission product yield experimental data; 3) Fission product yield evaluation; and 4) Fission product yield validation. Technical discussions and the resulting work plan of the Coordinated Research Programme are summarized in this report.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

Revision of Fission Yields Uncertainties in ENDF/B-VIII.0

The spontaneous and neutron-induced fission yield sublibraries in the Evaluated Nuclear Data Files (ENDF/B) contain cumulative and independent fission yield values for dozens of fissioning systems, and hundreds of fission products. In this work, we report on a correction step that was undertaken after observing anomalously large uncertainties for several end-of-chain fission products. A total of 17 cumulative fission yield uncertainties and the value of 2 independent yields were corrected as a result of this revision.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

Impact of fission yield covariance matrices on decay heat uncertainty quantification with the DARWIN2 package

Although fission yields are strongly correlated, correlations between them are usually not taken into account when performing decay heat uncertainty calculations with the CEA DARWIN2 package due to the lack of reference covariance matrices associated to the JEFF-3.1.1 evaluation. However, covariance matrices for {sup 235}U and {sup 239}Pu thermal fission yields have been produced recently by the subgroup 37 of OECD/NEA Working Party on International Nuclear Data Evaluation Cooperation (WPEC). The study presented in this paper evaluates the effect of those covariances on the decay heat uncertainty calculation, both on fission burst experiments and on integral decay heat measurements that are part of the DARWIN2 experimental validation database. Although some differences are observed, partly due to the variety of models used to produce the matrices, the propagation of fission yield covariances always leads to a reduction of the decay heat uncertainty for cooling time above 10 seconds, indicating that not taking them into account is a conservative hypothesis from a safety point of view. Nevertheless, the strong impact of those covariances on the decay heat uncertainty also highlights the need of documented and consistent fission yield uncertainties and correlation data. On top of that, all the covariance matrices used for this study represent the correlation between the physical model parameters, but none of them includes the experimental correlations. An evaluation of the experimental correlations would also be of strong interest for decay heat uncertainty calculations. (authors)

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2021

Updating Fission Yield Data for Applications (Summary Report)

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2014

Study of asymmetric fission yield behavior from neutron-deficient Hg isotope

A study of asymmetric fission yield behavior from a neutron-deficient Hg isotope has been conducted. The fission yield calculation of the neutron-deficient Hg isotope using Brownian Metropolis shape had showed unusual result at decreasing energy. In this paper, this interesting feature will be validated by using nine degree of scission shapes parameterization from Brosa model that had been implemented in TALYS nuclear reaction code. This validation is intended to show agreement between both model and the experiment result. The expected result from these models considered to be different due to dynamical properties that implemented in both models.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗