Prompt Fission Neutron Spectra Research Articles

EXFOR-based simultaneous evaluation for neutron-induced fission cross section of plutonium-242

ABSTRACT The 242Pu neutron-induced fission cross section was evaluated from 100 keV to 200 MeV. The experimental 242Pu and 235U fission cross sections and their ratios in the EXFOR library were reviewed and analysed by the least-squares method. Additional simultaneous evaluation was performed by including the experimental database of the 233,238U and 239,240,241Pu fission cross sections and their ratios developed for JENDL-5 evaluation. The 242Pu fission cross sections from our evaluation and JENDL-5 evaluation are close to each other below 1 MeV while they systematically differ from each other above 10 MeV. The cross section from our evaluation is systematically lower than the JENDL-4.0 cross section in the prompt fission neutron spectrum peak region (∼5% lower around 1 MeV). The newly evaluated 242Pu fission cross section was verified against the cross section measured in the 252Cf spontaneous fission neutron field and criticalities of small-sized LANL fast systems and demonstrated better performance than the JENDL-4.0 cross section on the same level with the JENDL-5 cross section.

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 235U 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, 235U and 239Pu PFNS were measured by Nicodemus and Staub. These also proved to be quite accurate and gave an average spectrum energy of 2 MeV for 235U. [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.

Study of 239Pu(n,f) prompt fission neutron spectrum

The experimental data concerning 239Pu prompt fission neutron spectrum above 10 MeV are sparse, and no spectrum averaged cross section has been measured in this neutron field yet. The first measurement was performed at the IBR-2 reactor, which uses plutonium dioxide fuel. The present work aimed at the measurement of spectral averaged cross sections for high threshold reactions such as 46Ti(n,p)46Sc, 54Fe(n,p)54Mn, 58Ni(n,X)57Co, 89Y(n,2n)88Y, and 209Bi(n,3n)207Bi to explore the high energy region of the 239Pu prompt fission neutron spectrum. Measurement of spectrum averaged cross section for the 89Y(n,2n)88Y reaction is included in NEA high priority request list. The 58Ni(n,p)58Co reaction was employed as a monitor reaction. The experimental spectral averaged cross sections were derived from reaction rates measured by means of high purity Germanium spectrometry. The experimental values were compared with spectrum averaged cross sections compiled from either ENDF/B-VIII.0, GMA or JEFF-3.3 239Pu prompt fission neutron spectrum and IRDFF-II cross sections. The best agreement, i.e. within uncertainties, was achieved using GMA 239Pu prompt fission neutron spectrum for all reactions under study. Calculation results using JEFF-3.3 and ENDF/B-VIII.0 evaluations of the 239Pu prompt fission neutron spectrum agree well with the experimental data except for the high energy region reflected in the disagreement with the 209Bi(n,3n)207Bi reaction.

Shedding light on the 239Pu fission source term with new high-precision experiments and advanced fission modeling

In the last decade, there has been a renaissance of fission research resulting in new high-precision experiments and advanced fission modeling. For instance, the Chi-Nu and CEA teams supplied, for the first time, the 239Pu prompt fission neutron spectrum (PFNS) for broad ranges of incident and outgoing neutron energies. The CEA team also measured 239Pu average prompt neutron multiplicities, ν̄p, with lower statistical uncertainties and a technique significantly different than the one used in the past. The NIFFTE collaboration provided 239Pu(n,f)/235U(n,f) cross section shape ratios with uncertainties below 1% utilizing a novel detector type. Advanced fission event generators were developed, among them CGMF, FIFRELIN, FREYA, and GEF, which calculate post-scission fission observables in a correlated manner. These new experimental data and more consistent fission models change the evaluated PFNS, ν̄p, and (n,f) cross sections, some only modestly, compared to ENDF/B-VIII.0. In turn, the individual new nuclear data distinctly change simulated effective neutron multiplication factors of fast critical assemblies, but their combined impact is small, while affecting the prediction of LLNL pulsed sphere neutron leakage spectra and reaction rates only within experimental uncertainties. Also, the parameters obtained from fitting to ν̄p reproduce various post-scission fission observables within the uncertainties of experimental data. This indicates that new differential experiments and consistent fission modeling reduce compensating errors present in ENDF/B-VIII.0.

Templates of expected measurement uncertainties for prompt fission neutron spectra

In this paper, we provide templates of uncertainty sources expected to appear for three measurement types of prompt fission neutron spectra (PFNS): (1) shape measurements, (2) clean-ratio shape, that is the monitor PFNS are measured in nearly exactly the same surrounding as the PFNS of interest, and (3) indirect ratios, where the detector efficiency is backed out from PFNS monitor measurements. Information is also listed that is needed to faithfully include PFNS in nuclear data evaluations to guide experimenters on how to best report data and metadata for their measurements. These templates also suggest a typical range of pertinent uncertainty values and their correlations in case realistic uncertainties cannot be estimated from information on the measurement itself. The templates were based on a literature review, information found in EXFOR for 252Cf, 235, 238U, and 239Pu PFNS, and enhanced by expertise from experimenters contributing to these PFNS templates.

EUCLID: A New Approach to Constrain Nuclear Data via Optimized Validation Experiments using Machine Learning

Compensating errors between several nuclear data observables in a library can adversely impact application simulations. The EUCLID project (Experiments Underpinned by Computational Learning for Improvements in Nuclear Data) set out to first identify where compensating errors could be hiding in our libraries, and then design validation experiments optimized to reduce compensating errors for a chosen set of nuclear data. Adjustment of nuclear data will be performed to assess whether the new experimental data—spanning measurements from multiple responses—successfully reduced compensating errors. The specific target nuclear data for EUCLID are 239Pu fission, inelastic scattering, elastic scattering, capture, nu-bar, and prompt fission neutron spectrum (PFNS). A new experiment has been designed, which will be performed at the National Criticality Experiments Research Center (NCERC).

Templates of expected measurement uncertainties

The covariance committee of CSEWG (Cross Section Evaluation Working Group) established templates of expected measurement uncertainties for neutron-induced total, (n,γ), neutron-induced charged-particle, and (n,xn) reaction cross sections as well as prompt fission neutron spectra, average prompt and total fission neutron multiplicities, and fission yields. Templates provide a list of what uncertainty sources are expected for each measurement type and observable, and suggest typical ranges of these uncertainties and correlations based on a survey of experimental data, associated literature, and feedback from experimenters. Information needed to faithfully include the experimental data in the nuclear-data evaluation process is also provided. These templates could assist (a) experimenters and EXFOR compilers in delivering more complete uncertainties and measurement information relevant for evaluations of new experimental data, and (b) evaluators in achieving a more comprehensive uncertainty quantification for evaluation purposes. This effort might ultimately lead to more realistic evaluated covariances for nuclear-data applications. In this topical issue, we cover the templates coming out of this CSEWG effort–typically, one observable per paper. This paper here prefaces this topical issue by introducing the concept and mathematical framework of templates, discussing potential use cases, and giving an example of how they can be applied (estimating missing experimental uncertainties of 235U(n,f) average prompt fission neutron multiplicities), and their impact on nuclear-data evaluations.

Prompt fission neutron spectra in the 235U(n,f) reaction

Prompt fission neutron spectra (PFNS) are crucial to any neutronic simulation of critical nuclear systems. An experimental setup dedicated to the measurements of PFNS of very high accuracy was developed at the Los Alamos Neutron Science Center (LANSCE) some ten years ago. It allows for the measurement of PFNS for neutron induced fission at the Weapon Neutron Research (WNR) neutron source of the LANSCE. A measurement of the PFNS from the 235U(n,f) reaction was realized recently and is currently analyzed. Preliminary results are presented here and are compared to present nuclear data evaluations.

Producing Evaluation-quality 239Pu Average Prompt Fission Neutron Multiplicities using a Correlated Fission Model

An evaluation of the average prompt fission neutron multiplicity, ν¯ p, of 239Pu(n,f) is shown. This evaluation includes (a) the correlated fission model CGMF, and (b) a detailed analysis of past and recently published experimental data. Using CGMF-calculated ν¯ pas prior enables to link, through the use of evaluated model input parameters, ν¯ p to other fission observables such as the prompt fission neutron spectrum (PFNS), pre-neutron emission fission yields as a function of mass, and the average total kinetic energy of the fragments. These evaluated parameters produce realistic predictions of many fission observables, while the evaluated ν¯ p agrees well (χ2 ≈ 1) with data. Moreover, with the new evaluated ν¯ p, the effective neutron multiplication factor of fast Pu ICSBEP critical assemblies are predicted with a mean bias of 58 pcm compared to 18 pcm with ENDF/B-VIII.0, when paired with a new 239Pu PFNS and fission cross section. Due to these encouraging validation results, the evaluated ν¯ p is currently part of a release candidate for the 239Pu ENDF/B-VIII.1 file. Hence, a correlated fission model was used for the first time for evaluating ν¯ p that is of evaluation quality. This is an important step towards consistent evaluations of prompt fission observables.

Experimental Prompt Fission Neutron Spectra Comparisons for the 235,238U(n, f) and 239Pu(n, f) Reactions

The Chi-Nu project to measure prompt fission neutron energy spectra for the major actinides has now completed two measurements, for neutron-induced fission of 239Pu and 235U for incident neutron energies from 1 to 20 MeV, and has almost completed the prompt fission neutron spectrum measurement for 238U. In addition, similar data have been taken for spontaneous fission in some other isotopes, and a measurement of fission neutron spectra from 240Pu(n, f ) is in progress. These measurements are done at the same facility, with the same equipment and analyzed in a similar way. A useful way to look at such data is to examine ratios of the prompt fission neutron spectra among actinides, as some of the experimental uncertainties involved in these data are the same from isotope to isotope, making the ratios of fission neutron spectra less dependent on the experimental and analysis details. We discuss here the ratios of prompt fission neutron spectra between 239Pu(n, f ) and 235U(n, f ) , as well as the evolution of the mean fission neutron energy for 239Pu(n, f ) and 235,238U(n, f ) with increasing incident neutron energy.

The Covariance of PFNS Results from the Chi-Nu Experiment

The prompt fission neutron spectrum (PFNS) from neutron-induced fission is a fundamental quantity for the behavior of nuclear reactors, and has been measured many times on a wide variety of nuclei and covering different ranges of incident and emitted neutron energies. However, results from past measurements are frequently called into question in modern nuclear data evaluations because of a lack of thorough experimental documentation and incomplete uncertainty analyses. The Chi-Nu experiment at Los Alamos National Laboratory was designed to produce high-precision measurements of the PFNS of major actinides over a wide range of incident and emitted neutron energies, and with the documentation and covariance analysis required to ensure that the results of this experiment maintain their impact long into the future, thereby avoiding this pitfall of past measurements. In this work we describe the Chi-Nu experiment along with summaries of the treatment of and methods developed to address two important components of the analysis of Chi-Nu data: random-coincidence backgrounds and MCNP simulations. Furthermore, we describe the first results for correlations not just between all data points collected on a single target nucleus, but also between all data points from separate Chi-Nu measurements on 235U and 239Pu. These correlations are important for accurately calculating ratios of the PFNS from one actinide to another, which are rare and can be informative for nuclear data evaluation efforts.

Method to Compare Fission-to-Scattering Ratios using Uranium-238

A novel method was developed to separate the 238U fission contribution measured in quasi-differential time-of-flight scattering experiments in order to isolate the elastic and inelastic events. Pulse height distributions from in-beam measurements were used to generate response functions, which were used to reconstruct the 238U prompt fission neutron spectra. This method was validated by reconstructing the measured 252Cf spontaneous fission pulse height distribution. Monte Carlo calculations were used to model the experiment. Good agreement was observed between the measured and calculated 238U fission contribution.

Impact of reactor neutron spectrum on measured spectrum averaged cross sections

The cross section averaged over 235U thermal-neutron induced fission spectrum is a fundamental quantity that can be used in evaluation and validation of nuclear data. Many experiments focused on the determination of Spectrum Averaged Cross Sections (SACS) in 235U(nth,f) Prompt Fission Neutron Spectrum (PFNS) in light water reactors using enriched uranium fuel. In these reactors, there is already some amount of water moderator between the uranium fuel and the irradiated sample. Due to the decrease of hydrogen cross-section with neutron energy, the high energy tail of the reactor spectrum in cores with water moderator may be harder than the pure PFNS. This paper aims to compare the shape of the actual reactor spectrum in various core positions of a research light-water reactor differing each from other by the effective water thickness. The spectrum shape is determined both by calculations and experimentally using various high energy threshold reactions.The impact of the photo-nuclear reactions (γ,n) competing with (n,2n) in production of the same residual nucleus was shown to be less than a percent for most of studied dosimeters. An important exception was found for 197Au(n,2n)196Au dosimeter irradiated in the outcore channel where a notable photo-neutron contribution to the production of 196Au is caused by the neutron production from the high energy γ-rays from thermal-neutron capture in 54Fe. The corresponding ENDF/B-VIII.0 data turned out to underestimate such γ-yield by 40 % in comparison with ENDF/B-VI.8. This has improved but however not resolved the disagreement between our measurement and calculations. The remaining deficiency was attributed to the underestimation of the evaluated cross section IAEA/PD-2019 for the 197Au(γ,n) cross section near the reaction threshold. The later was confirmed by comparison with existing measured data.

Measurement of the U235(n,f) prompt fission neutron spectrum from 10 keV to 10 MeV induced by neutrons of energy from 1 MeV to 20 MeV

The characterization of fission-driven nuclear systems primarily relies on calculations of neutron-induced chain reactions, and these calculations require evaluated nuclear data as input. Calculation accuracy heavily depends on input nuclear data evaluation accuracy, and thus high precision on the experimental input to the nuclear data evaluation is essential for fundamental quantities like the energy spectrum of neutrons emitted from neutron-induced fission (i.e., the prompt fission neutron spectrum, PFNS). Despite decades of measurement efforts, prior to the measurements described in this work there were only three literature data sets for the $^{235}\mathrm{U}(n,f)$ PFNS at incident neutron energies above 1.0 MeV considered reliable for inclusion in nuclear data evaluations and no reliable data sets above 3.0 MeV incident neutron energy. In this work we report on new measurements of the $^{235}\mathrm{U}(n,f)$ PFNS spanning a grid of 1.0--20.0 MeV in incident neutron energy and 0.01--10.0 MeV in outgoing (PFNS) neutron energy. These measurements were carried out at the Weapons Neutron Research facility at the Los Alamos Neutron Science Center and used a multifoil parallel-plate avalanche counter target with both a Li-glass and a liquid scintillator detector array in separate experiments to span the quoted outgoing neutron energy ranges. The PFNS results are shown in terms of the energy spectra themselves as well as the average PFNS energy ($\ensuremath{\langle}E\ensuremath{\rangle}$) and ratios of $\ensuremath{\langle}E\ensuremath{\rangle}$ at forward and backward angles. The results are compared with literature data and selected nuclear data evaluations. Generally, the data agree with the ENDF/B-VIII.0 evaluation below 5.0-MeV incident neutron energy and more closely with the JEFF-3.3 evaluation above 5.0 MeV, though no evaluations considered for comparison in this work agree with the data across all of the incident and outgoing neutron energies shown, especially in regions where the third-chance fission process becomes available. Additionally, we show a ratio of the present PFNS results for $^{235}\mathrm{U}(n,f)$ with a recent and highly correlated experiment to measure the $^{239}\mathrm{Pu}(n,f)$ PFNS at the same experimental facility and with nearly identical equipment and analysis procedures. Many observations reported in this work are the first of their kind and represent significant advancements for knowledge of the $^{235}\mathrm{U}(n,f)$ PFNS.

Characterization of the neutron/[formula omitted]-ray discrimination performance in an EJ-301 liquid scintillator for application to prompt fission neutron spectrum measurements at CSNS

The FIssion Neutron spectrum Detector Array (FINDA) has been designed for measurement of prompt fission neutron spectrum on the Back-n beam line at the China Spallation Neutron Source (CSNS). In order to test the neutron-γ discrimination performance of the EJ301 scintillator that will be used as a detector unit in the FINDA, a comparative study using three conventional digital pulse shape discrimination (PSD) methods has been carried out. An Am–Be source has been used to generate the mixed neutron-γ radiation and the waveform data has been obtained with a fast digitizer. Pulse interpolation, baseline restoration and pulses pile-up rejection have been applied for digital pulse processing. Charge comparison (CC) method and simplified charge comparison(SCC) method show a better capability of neutron-γ discrimination than rise time comparison(RTC) method over the entire energy range. Rise time comparison method needs a very fast digitizer or pulse interpolation to improve the PSD ability. The analysis of neutron-γ discrimination performance of the EJ301 scintillator provides a strong technical support for fast neutron measurement using the FINDA at CSNS.

Systematic Distortion Factor and Unrecognized Source of Uncertainties in Nuclear Data Measurements and Evaluations

Each experiment provides new information about the value of some physical quantity. However, not only measured values but also the uncertainties assigned to them are an important part of the results. The metrological guides provide recommendations for the presentation of the uncertainties of the measurement results: statistics and systematic components of the uncertainties should be explained, estimated, and presented separately as the results of the measurements. The experimental set-ups, the models of experiments for the derivation of physical values from primary measured quantities, are the product of human activity, making it a rather subjective field. The Systematic Distortion Factor (SDF) may exist in any experiment. It leads to the bias of the measured value from an unknown “true” value. The SDF appears as a real physical effect if it is not removed with additional measurements or analysis. For a set of measured data with the best evaluated true value, their differences beyond their uncertainties can be explained by the presence of Unrecognized Source of Uncertainties (USU) in these data. We can link the presence of USU in the data with the presence of SDF in the results of measurements. The paper demonstrates the existence of SDF in Prompt Fission Neutron Spectra (PFNS) measurements, measurements of fission cross sections, and measurements of Maxwellian spectrum averaged neutron capture cross sections for astrophysical applications. The paper discusses introducing and accounting for the USU in the data evaluation in cases when SDF cannot be eliminated. As an example, the model case of 238U(n,f)/235U(n,f) cross section ratio evaluation is demonstrated.

Uncertainty propagation of prompt fission neutron spectrum for physics analysis of fast and thermal reactors

This paper presents a strategy for processing the covariance matrix of the prompt fission neutron spectrum (PFNS) and propagating the PFNS uncertainties to the neutronic calculation of fast and thermal reactors. Due to their great significance to the accurate prediction of nuclear criticality, the sensitivity and uncertainty of core parameters for PFNS are analyzed in this study. The propagation of PFNS uncertainties from the evaluated nuclear data files (ENDF) to the core parameters is divided into two phases. In the first phase, the covariance data in the ENDF is transformed into the multi-group form, in which the “zero-sum” constraint is considered and a corresponding functional module is developed in the updated NECP-Atlas nuclear data processing code. In the second phase, the neutron transport code is coupled as a “black box” to propagate the uncertainties in the multi-group form to the core parameters. Sensitivity and uncertainty (S&U) analysis function is implemented in the NECP-UNICORN uncertainty quantification code. As for its application, S&U analysis for PFNS has been performed to the fast and thermal reactors. The numerical results indicate that the influence of PFNS uncertainties to the confidence interval of reactivity prediction and power distribution should be considered in the nuclear reactor analyses.

ATHENA: A unique radiation environment platform at the National Ignition Facility

This paper describes the ATHENA platform, an energy tuning assembly, which was developed to spectrally shape the National Ignition Facility (NIF) deuterium–tritium fusion neutron source to a thermonuclear (fusion) plus prompt fission neutron spectrum with a capability to act as a short-pulse neutron source. This unique, otherwise inaccessible radiation environment complements existing experimental facilities and capabilities. The flexible ATHENA irradiation positions were modeled using an ensemble of Monte Carlo simulations with stochastic sampling of the nuclear cross-sections to characterize the radiation environments and uncertainty for the platform. Validation of the internal neutron spectrum produced from fielding ATHENA at NIF occurred through neutron flux unfolding with 20 measured activation products. The STAYSL unfolded neutron flux resulted in a reduced χ2 value of 1.4 with a larger contribution from 46Ti(n,2n) reaction channel. The total ionizing dose was measured to be 515 ± 7.9% rad(TLD-400), whereas the modeled values indicated a lower value of 290 ± 4.6% rad(TLD-400). The NIF experiment demonstrated that ATHENA is capable of producing a thermonuclear and prompt fission neutron spectrum with a 50 nanosecond pulse width and a 1-MeV equivalent neutron fluence of 3.6×1012ncm2 with strong radial uniformity over the sample volume. Example case studies of ATHENA for integral experiments and microelectronic device responses are also presented.

Progress on the reevaluation and validation of the n+233U neutron cross sections

The set of 233U resonance parameters of the ENDF/B-VIII.0 nuclear data library was adopted from the previous ENDF/B-VII.1 evaluation using the external levels to update the thermal values. Adoption of IAEA 2017 thermal standards (σf=533.0±2.2 b, σc=44.9±0.9 b, and ν‾tot=2.487±0.011) and of the IAEA-recommended thermal-neutron induced prompt fission neutron spectrum (PFNS) with average PFNS energy of 2.030±0.013 MeV requires a re-evaluation of 233U neutron cross sections in the resolved resonance region. A newly produced evaluation is being tested on benchmarks carefully selected from the Handbook of International Criticality Safety Benchmark Experiments (ICSBEP) which are highly sensitive to 233U data. An important goal of this work was to eliminate the strong negative gradient of the calculated effective multiplication factors with respect to the epithermal fission fraction observed in the validation of the ENDF/B-VIII.0 library for those assemblies. A significant improvement in integral performance of critical 233U solutions is observed for the newly proposed evaluation. Further work addressing the fast neutron region is needed.

Influence of nonstatistical properties in nuclear structure on emission of prompt fission neutrons

The Hauser-Feshbach Fission Fragment Decay (HF$^3$D) model is extended to calculate the prompt fission neutron spectrum (PFNS) for the thermal neutron induced fission on $^{235}$U, where the evaporated neutrons from all possible fission fragment pairs are aggregated. By studying model parameter sensitivities on the calculated PFNS, as well as non-statistical behavior of low-lying discrete level spin distribution, we conclude that discrepancies between the aggregation calculation and the experimental PFNS seen at higher neutron emission energies can be attributed to both the primary fission fragment yield distribution and the possible high spin states that are not predicted by the statistical theory of nuclear structure.