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DOE OSTI2022

Energy-dependent optimization of the prompt fission neutron spectrum with CGMF

Throughout the course of FY21, significant effort was put into investigating models within the LANL developed Hauser-Feshbach fission fragment decay code, CGMF, to understand and potentially solve the long-standing challenge of a too-soft prompt fission neutron spectrum, PFNS. Several inputs and models to CGMF were investigated, including the discrete nuclear levels, the optical model potential, level densities, and the fission fragment initial conditions. Some of the global models within CGMF led to a slight hardening of the neutron spectrum—particularly the likely incomplete discrete levels in through which γ-rays decay—but none of the changes where large enough for the tail of the PFNS to reproduce experimental data. A significant hardening of the spectrum tail was observed when the fission fragment initial conditions were optimized based on their sensitivities to the PFNS data for thermal incident neutrons. In this way, the parameters for the CGMF mass and total kinetic energy distributions, along with the spin cutoff factor were adjusted to better reproduce the experimental PFNS measurements. This optimization hardened the tail of the PFNS slightly but led to unphysical mass distributions for the fission fragments before neutron emission. It was clear from the above that we do not expect to be able to produce an evaluation-quality PFNS with CGMF in the near future. Challenges at thermal will persist–and possibly worsen–with increasing incident energy, where more models are needed to completely describe the fission. Basic-science research funding exceeding the amount available and scope of our NCSP funds would be needed to tackle this decade-long challenge impacting many fission-fragment event generator. And, in fact, Amy Lovell won LDRD ECR funding to do so over the next few years. Therefore, we focused in FY22 on extending evaluation capabilities beyond thermal incident neutrons, to take into account the incident energy dependence of the PFNS and fission fragment initial condition distributions in CGMF. We chose to set up the evaluation methodology to perform PFNS evaluations with CGMF across incident-neutron energies, in order to have it readily available for future NCSP evaluations when the PFNS from CGMF has improved. In this report, we outline the evaluation methodology, along with the results of the optimization, including full model calculations with CGMF using the evaluated parameters.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Measurement of the Prompt Fission Neutron Spectrum from 800 keV to 10 MeV for 240 Pu($sf$) and for the 240 Pu($n,f$) Reaction Induced by Neutrons of Energy from 1-20 MeV

The presence of 240 Pu in nuclear fuels for reactors has resulted in high uncertainties in the results of reactor and nuclear transmutation calculations because of deficiencies in 240 Pu-related nuclear data. Specifically for the prompt fission neutron spectrum (PFNS) of 240 Pu, there is only one neutron-induced, ($n,f$), measurement at 0.85 MeV incident neutron energy and only one complete spontaneous fission, ($sf$), measurement. This limited availability of data does not sufficiently guide nuclear data evaluations of these quantities. Here we report on a measurement of both the 240 Pu($sf$) and the 240 Pu($n,f$) PFNS, both over the emitted neutron energy range of 0.79–10.0 MeV, and from incident neutron energies of 1.0–20.0 MeV for the ($n,f$) reaction. Measurements were made with a hemispherical array of liquid scintillators at the high-energy Los Alamos Neutron Science Center white neutron source at the Weapons Neutron Research facility as part of the joint LANL-LLNL Chi-Nu experimental campaign to measure actinide fission neutron spectra. These measurements are the first of their kind, and provide clear experimental evidence for second-chance fission, third-chance fission, and pre-equilibrium neutron emission processes in neutron-induced fission of 240 Pu, and are the first ever measurements above 1 MeV incident neutron energy.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

AIACHNE's contribution for Nuclear Energy Agency Working Party on International Nuclear Data Evaluation Co-operation Subgroup 50

The AIACHNE (AI/ML Informed cAlifornium CHi Nuclear data Experiment) project aims at designing an experiment for the 252 Cf Prompt Fission Neutron Spectrum (PFNS) that explores systematic biases in an experimental database retrieved from the EXFOR databases. To that end, machine learning (ML) methods were applied to pint-point measurement features likely related to bias. From that information, we selected a feature that should be explored by the AIACHNE experiment. Measurement features are metadata encapsulating all pertinent information about the physical measurement and analysis techniques. Examples are, for instance, what neutron and fission detectors were used for the physical metadata, and what background reduction techniques were employed for analysis techniques. Such metadata were retrieved both from EXFOR entries as well as the literature of data sets described in detail in Reference 2 (at the end of the article).

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

AIACHNE's contribution for Nuclear Energy Agency Working Party on International Nuclear Data Evaluation Co-operation Subgroup 50

The AIACHNE (AI/ML Informed cAlifornium CHi Nuclear data Experiment) project aims at designing an experiment for the 252 Cf Prompt Fission Neutron Spectrum (PFNS) that explores systematic biases in an experimental database retrieved from the EXFOR databases. To that end, machine learning (ML) methods were applied to pint-point measurement features likely related to bia. From that information, we selected a feature that should be explored by the AIACHNE experiment. Measurement features are metadata encapsulating all pertinent information about the physical measurement and analysis techniques. Examples are, for instance, what neutron and fission detectors were used for the physical metadata, and what background reduction techniques were employed for analysis techniques. Such metadata were retrieved both from EXFOR entries as well as the literature of data sets described in detail in Ref. [2]. The prerequisite for applying machine learning techniques is casting the metadata into a format that can be parsed by the algorithm. This step might seem trivial but requires to find a unique language where metadata that carry the same physics meaning across several experiments must have the same identifier. One example is, for instance, the neutron detector. As seen in Figure 1, the machine learning code identified the use of 6 Li detectors as being related to bias in some datasets of the AIACHNE 252 Cf PFNS experimental database. In fact, here are several experiments that used neutron detectors containing 6Li in the database, for instance for the example below. EXFOR format has a unique keywords describing detectors such as “SCIN” or “GLASD”. One may think that these keywords are already sufficient descriptors for ML to uniquely find an issue. However, “SCIN” (used for [3, 4]) and “GLASD” (used for [5]) fail to inform the algorithm what is the active material in the detector. And, the key common issue leading to bias in 252 Cf related to neutron detectors is not whether it is a glass detector or a scintillator. No, the issue is that 6 Li was within both detector types and that even small mistakes in the detector response functions around approximately 200 keV are amplified by the 6 Li(n,α) resonance there leading to bias in data as highlighted in Fig. 1 and Ref. [1]. Hence, the features describing the neutron detector must call out the active material in the detector, rather than the existing EXFOR detector keyword, that the ML algorithm can find physically meaningful features related to bias. The AIACHNE team used a precursor of the WPEC (Working Party on International Nuclear Data Evaluation Co-operation) SG(Subgroup)-50 format to store the metadata for the ML analysis.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Manhattan Project 1940s research on the prompt fission neutron spectrum

We describe how the prompt fission neutron spectrum (PFNS) was determined for the Manhattan Project at Los Alamos. Early work before World War II at American and British universities is described, together with theoretical work by Feather at Cambridge and Bethe at Los Alamos. As the Manhattan Project was being planned in 1942, two experiments on natural uranium were commissioned that proved to be influential: 1) An integral experiment at Chicago by Christy and Manley that accurately determined the average PFNS spectrum energy, 2.2 ± 0.2 MeV; 2) Bloch and Staub’s Stanford cyclotron measurement of the PFNS spectrum, which obtained an average energy of 1.70 ± 0.34 MeV. These two papers, previously unavailable outside of Los Alamos, are reproduced in the Supplementary Appendix. From these data, at the beginning of the project in 1943 Serber estimated an average 235 U PFNS energy of 2 MeV, and indeed this agrees with today’s best estimate. The challenges facing the scientists involved both the availability of only very small samples of enriched uranium and plutonium targets, and fast neutron detection technologies. During the project, 235 U and 239 Pu PFNS were measured by Nicodemus and Staub. These also proved to be quite accurate and gave an average spectrum energy of 2 MeV for 235 U. [This is not reproduced in the Appendix because it was published after the war in Physical Review 89, 1288 (1953)]. New methods were developed to enable more accurate measurements, and this paper describes how the PFNS was determined surprisingly well by 1945. We end by describing the post-war measurements in the 50s, including the PFNS data used by Ford and Wheeler in their simulations in 1951, the Bonner 1952 data, the seminal 1952 Watt paper with a new empirical parametrization of the PFNS, and the accurate PFNS measurement undertaken at Los Alamos by Cranberg et al. in 1956. We compare the measurements with our best understanding today as embodied in the Evaluated Nuclear Data File ENDF/B-VIII.0. Some images from historical documents in our Los Alamos National Security Research Center (NSRC) archives are shown.

96 KNOWLEDGE MANAGEMENT AND PRESERVATION↗
DOE OSTI2022

239 Pu R -matrix Analysis and Neutron Multiplicities in the Neutron Energy Region up to a few keVs [Abstract]

The evaluation of 239 Pu neutron resonance parameters coupled to neutron multiplicities $\overline{v}_p$ is of particular importance to investigate the ($\mathcal{n, γf}$) reaction in which a $\mathcal{γ}$-ray emission occurs before the scission of the compound nuclear. This reaction has offered one explanation for the fluctuations in the measured values of $\overline{v}_p$ In this regard, the competition between ($\mathcal{n, γf}$) reaction and the direct fission process can be also included in the R matrix analysis of fission and capture measured data. The goal of this work is the coupled evaluation of the $\mathcal{n}$+ 239 Pu resonance parameters and related neutron multiplicities by ensuring the adoption of thermal neutron constants recently evaluated at the International Atomic Nuclear Energy as well as the recommended (thermal-neutron) induced prompt neutron fission spectrum (PFNS). Moreover, this new set of physical evaluated quantities should also guarantee the agreement for high-leakage solution benchmarks while keeping the good performance of large thermal solution assemblies.

07 ISOTOPE AND RADIATION SOURCES↗
DOE OSTI2023

Criticality Experiments to Reduce Compensating Errors in Plutonium Nuclear Data

Compensating errors between nuclear data observables in a library can adversely impact application simulations. The primary goal of the EUCLID project (Experiments Underpinned by Computational Learning for Improvements in Nuclear Data) is to reduce compensating errors in nuclear data. A new criticality experiment, described in this work, was designed with the specific target nuclear data of 239 Pu fission, inelastic scattering, elastic scattering, capture, nu-bar, and prompt fission neutron spectrum (PFNS). This work will focus on the design and execution of the EUCLID experiment, performed on the Planet vertical lift critical assembly machine at the National Criticality Experiments Research Center (NCERC). The criticality experiment includes two different configurations with very different geometries: one is cube-like to minimize neutron leakage while the other is slab-like to maximize leakage. Having these two widely varying configurations allows the scattering sensitivities of 239 Pu to the neutron multiplication factor to be greatly changed while minimally impacting the other cross section sensitivities. Both configurations utilize the Pu ZPPR (Zero Power Physics Reactor) plates as fuel. The experiments were designed using a D-Optimality criteria, which is an optimization method minimizing the log-determinant of the adjusted nuclear data covariance for the target reactions. These experiments include not only inference of k eff , as done in all critical benchmark experiments, but several other responses as well, such as neutron multiplication measurements and reaction rate ratios. After analysis of the measured data is complete, adjustment of nuclear data will be performed to assess whether the new experimental data successfully reduced compensating errors.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2024

The Prompt Fission Uranium Neutron Spectrum (PFUNS) Experiment: Critical Configurations and Irradiations

The objective of the Prompt Fission Uranium Neutron Spectrum (PFUNS) experiment is to reduce the uncertainty of the Prompt Fission Neutron Spectrum (PFNS) of 235 U above 8 MeV. The experiment was performed at the DOE National Criticality Experiments Research Center (NCERC) at the Nevada National Security Site. To meet the experiment objective, activation foils were placed in a central void region of a critical configuration consisting of concentric highly enriched uranium (HEU) metal hemishells. The set of activation foils were chosen based on threshold reactions to neutron energies across the fission spectrum, but especially those in the high energy tail of the fission spectrum. PFUNS was performed on the Planet critical assembly machine at NCERC and uses the Rocky Flats (RF) HEU hemishells. PFUNS has similarities to the Measurement of Uranium Subcritical and Critical (MUSiC) experiment conducted at NCERC in 2021, which also used RF hemishells, but contains a large central cavity to allow for a sample plate to be inserted. This large void means that much more HEU is needed to achieve a critical configuration (108 kg for PFUNS versus 59 kg for MUSiC). This work describes the 2024 experiment execution of four critical configurations and two irradiations for the PFUNS project.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Status, Challenges, and Plans for Consistent Modeling and Evaluation of Fission Data: Nubar, PFNS, and FPY [Slides]

This presentation discusses the importance of consistent evaluations for fission observables. Currently, prompt fission quantities (e.g., neutron multiplicity, neutron energy spectrum, and fission product yields) are evaluated independently of one another, either with separate models or data-only/non-model evaluations (few – if any – shared model inputs) and inconsistencies can arise in evaluated data (e.g. NSE 190, 258 (2018)). They have found that consistent, model-based evaluations lead to more physical constraints on free parameters in the model, more robust predictions for other observables and other isotopes, that there are correlations between the uncertainties on different observables, and that uncertainties can be propagated to unmeasured quantities. They are working on developing models to the point where fission observables are calculated at the quality needed for an evaluation. They are striving to consistently calculate fission observables, such as $\bar{v}$, PFNS, and FPY, to a quality suitable for an evaluation. Current evaluations for fission observables use separate models for each observable (with minimal shared input) or are purely data driven. LANL models, such as the Monte Carlo CGMF and deterministic BeoH, have different strengths; the similar fission fragment initial conditions and decay models leads to consistency between the two codes (FPY can be connected to $\bar{v}$ and PFNS, even when calculated by different codes). Work is underway by Lovell to optimize the models and Neudecker is working to perform detailed uncertainty quantification. The PFNS, in particular, presents a significant challenge.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Measurement of the 240 Pu(n,f) Prompt Fission Neutron Spectra with Chi-Nu

The DOE Nuclear Criticality Safety Program has funded a multi-year effort to measure the 240 Pu(n,f) Prompt Fission Neutron Spectrum at Chi-Nu. This project is a joint LANL-LLNL effort, involving the preparation of 12 240 Pu foils and construction of a Parallel-Plate Avalanche Counter at LLNL, with subsequent measurements of the 240 Pu(n,f) PFNS at the Chi-Nu beamline at the Los Alamos Neutron Science Center’s Weapons Neutron Research facility (LANSCE/WNR). We expect the PPAC to be ready in time to perform the measurements this run cycle.

240Pu Foils↗
DOE OSTI2022

Including Chi-Nu 235 U PFNS Experimental Data into an ENDF/B-VIII.1 Release Candidate Evaluation

This report documents an evaluation of 235 U prompt fission neutron spectra (PFNS) that is a release candidate for the upcoming U.S. nuclear data library, ENDF/B-VIII.1. This evaluation differs from its predecessor, ENDF/B-VIII.0, mainly by the inclusion of 235 U PFNS measured by the Chi-Nu team of LANL and LLNL. This data set is the first one that covers the 235 U PFNS for continuous incident-neutron energies of 1⁻20 MeV and outgoing-neutron energies from 10 keV⁻10 MeV with high precision. Previous data sets were either measured in a limited energy range or with less precision. Hence, these new Chi-Nu data provide decisive information for the evaluation. The resulting evaluated data correspond well to the new experimental PFNS. The evaluated PFNS also produce average mean energies and 239 Pu/ 235 U PFNS in agreement with associated Chi-Nu data. If one uses the new evaluated data to predict the neutron multiplication factor, k eff , of selected ICSBEP critical assemblies, the differences of simulated values compared to those using ENDF/B-VIII.0 is modest (less than 55 pcm). This difference in k eff can be easily accommodated by changes in the 235 U average prompt fission neutron multiplicity that is currently being re-evaluated. In addition to that, the new PFNS predict on average 235 U LLNL pulsed-sphere neutron-leakage spectra better than ENDF/B-VIIII.0 PFNS.

235U↗
DOE OSTI2024

Evaluating the 238 U PFNS Including Chi-Nu Experimental Data

This report documents an evaluation of 238 U prompt fission neutron spectra (PFNS) which is a deliverable for a FY2024 Q4 NCSP (Nuclear Criticality Safety Program) milestone. This evaluation is new; its prior input is based on extended Los Alamos and exciton models implemented in the code CoH. Experimental covariances were estimated for five experimental data sets. One of these data sets that was measured by the Chi-Nu team of LANL and LLNL. It covers the 238 U PFNS for continuous incident-neutron energies of 1–20 MeV and outgoing-neutron energies from 10 keV– 10 MeV with high precision. Contrary to Chi-Nu data, previous data sets were measured in a limited energy range. The resulting evaluated data correspond well to the experimental PFNS taken into account for the evaluation. The evaluated PFNS also produce average mean energies in agreement with associated Chi-Nu data. If one uses the new evaluated data to predict the neutron multiplication factor, k eff , of the Flattop, Flattop-Pu and BigTen ICSBEP critical assemblies (which all have thick reflectors with high percentages of 238 U), the differences of simulated values compared to those using ENDF/B-VIII.1β3 is modest (less than 25 pcm). In addition to that, the new PFNS predict on average 238 U LLNL pulsed-sphere neutron-leakage spectra slightly better than ENDF/BVIIII.0 and ENDF/B-VIII.1β3 PFNS. The differences are, however, well within the experimental uncertainties.

238U↗
DOE OSTI2022

Evaluated 238 U(n,f) Average Prompt Fission Neutron Multiplicities Including the CGMF Model

This report documents an evaluation of the average prompt fission neutron multiplicity, $\overline{v}_p$, of 238 U from 800 keV to MeV. This evaluation had to be re-done from “scratch” as the input to previous $\overline{v}_p$ evaluations, specifically ENDF/B-VIII.0, was not found. That means that all available experimental data were re-analyzed and uncertainties were re-estimated. The new evaluated 238 U $\overline{v}_p$ based on only experimental data differs distinctly from ENDF/B-VIII.0 $\overline{v}_p$ from 2 to 4.5 MeV, and from 6 to 7 MeV, and is otherwise similar. The difference from 2 to 4.5 MeV stems from the fact that ENDF/B-VIII.0 was tweaked in this energy range to data of Frehaut, while two other, equally trustworthy, data sets would indicate an evaluated 238 U $\overline{v}_p$ that is up to 2% higher. Also, second chance fission in ENDF/B-VIII.0 was smoothed over from 6–7 MeV. Another major difference to ENDF/B-VIII.0 is that one of the evaluations presented here includes model information from the Hauser-Feshbach fission fragment decay code CGMF, while ENDF/B-VIII.0 is based purely on experimental data. CGMF links several fission quantities with each other; $\overline{v}_p$ is predicted by assumptions made on, e.g., pre-neutron emission yields as a function of mass, the total kinetic energy, or spin and parity of fission fragments. This allows to validate the new 238 U $\overline{v}_p$ by using CGMF parameters obtained from fitting to experimental 238 U $\overline{v}_p$ to predict yields as a function of mass, the average total kinetic energy, or the mean energy of the prompt fission neutron spectrum. These model-predicted values can then be compared to experimental and evaluated data. The model-predicted fission-observable values using evaluated parameters obtained here are reasonably close to experimental data for some observables, but are farther away from experimental data related to TKE observables. In addition to that, the evaluated 238 U(n,f) $\overline{v}_p$ shows similar deviations from ENDF/B-VIII.0 as for the evaluation with only experimental data. This difference is expected to lead to changes in simulated effective neutron multiplication factor, $k_{eff}$ of ICSBEP critical assemblies that are sensitive to 238 U in the fast range (BigTen, Flattop, Flattop-Pu). These changes in $k_{eff}$ need to be counter-balanced. Chi-Nu PFNS experimental data are expected to be released in the next few months that might lead to the needed changes in the PFNS. Until then, we hold off in benchmarking the new 238 U(n,f) $\overline{v}_p$ as well as submitting it to ENDF/B-VIII.1. Also, new high-precision 238 U $\overline{v}_p$ are expected to be measured by the CEA in the next two years that will shed further light on question on 238 U $\overline{v}_p$ from 2–4.5 and 6–7 MeV.

238U↗