Prompt fission neutron spectra for neutron-induced fission of Pu-239 and U-235
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Integral neutronics experiments have been a powerful tool and method for examining the reliability of evaluated nuclear data. In the present paper, the accuracy of evaluated nuclear data for Zirconium has been validated by comparing measured leakage neutron spectra with calculated ones. Leakage neutron spectra from the irradiation of D-T neutrons on Zirconium samples were experimentally measured at 60° and 120° by using a time-of-flight method. Theoretical calculations are carried out by Monte Carlo neutron transport code MCNP-4C with evaluated nuclear data of the ENDF/B-VII.0, ENDF/B-VIII.0, JENDL-4.0 and CENDL-3.1 libraries. From the comparisons, it is found that the calculations with JENDL-4.0 gives better agreements with the experiments at 60° while a large discrepancies are observed in the 4–13.5 MeV energy range at 120°. However, the calculated spectra using the data from ENDF/B-VII.0, ENDF/B-VIII.0 and CENDL-3.1 libraries showed some discrepancies with the measured ones, especially caused by the difference of the elastic and inelastic angular distributions and the secondary neutron energy distributions in the continuum inelastic scattering.
The Scale Method was applied for an analysis of experimental and evaluated data of Prompt Fission Neutron Spectra for different isotopes and incident neutron energies below 6 MeV. It was demonstrated that the method describes all experimental data sets in the outgoing neutron energy range 0–7 MeV within uncertainties. Theoretical arguments were provided to support the application of this method. Some important peculiarities connected with the neutron emission mechanism were identified, and proposals for future theoretical and experimental investigations were discussed. It was concluded that the new evaluations completed recently for {sup 235}U systematically overestimate the average energy of experimental prompt fission neutron spectra.
Prompt-fission-neutron spectra from Pu 239 ( n , f ) were measured with respect to Cf 252 spontaneous fission for incident neutron energies from 0.7 to 700 MeV at the Weapons Neutron Research facility (WNR) of the Los Alamos Neutron Science Center. A newly designed high-efficiency fission chamber was coupled to the highly segmented Chi-Nu neutron liquid scintillator array to detect neutrons emitted in fission events. The double time-of-flight technique was used to deduce the incident neutron energies from the spallation target and the outgoing-neutron energies from the fission chamber. Prompt-fission-neutron spectra (PFNS) were measured with respect to Cf 252 spontaneous fission down to 200 keV and up to about 12 MeV for all the incident neutron energies with typical total uncertainties well below 2 % up to about 7-MeV outgoing-neutron energy. The general trend of PFNS is well reproduced by JEFF3.3 and ENDF evaluations, although a better agreement is found with JEFF3.3. Discrepancies were observed for the low-energy part of the spectra, especially around the opening of the second-, third- and fourth-chance fission. Additionally, neutron average kinetic energies as a function of incident neutron energy are obtained experimentally with reported total uncertainties below 0.5 % . The measured values agree with the most recent data. The trend is fairly well reproduced by the JEFF3.3 evaluation, although it fails to reproduce the experimental values within their uncertainties.
Scattered neutron spectroscopy is a diagnostic technique commonly used to measure areal density in inertial confinement fusion experiments. Deleterious areal density asymmetries modify the shape of the scattered neutron spectrum. In this work, a novel analysis is developed, which can be used to fit the shape change. This will allow experimental scattered neutron spectroscopy to directly infer the amplitude and mode of the areal density asymmetries, with little sensitivity to confounding factors that affect other diagnostics for areal density. The model is tested on spectra produced by a neutron transport calculation with both isotropic and anisotropic primary fusion neutron sources. Multiple lines of sight are required to infer the areal density distribution over the whole sphere—we investigate the error propagation and optimal detector arrangement associated with the inference of mode 1 asymmetries.
Measurements of the areal density (ρR) of inertially confined implosions are critical to evaluate their performance. On OMEGA, ρR is inferred from measurements of the scattered neutron spectrum via neutron-time-of-flight (nTOF) and magnetic recoil spectrometer detectors. The nTOF measurements, in particular, have the ability to measure a wide range of neutron energies and thus scattering angles, with high precision. However, the neutrons that are backscattered into the detector must transit through the entire dense fuel assembly, and as a result are subject to rescattering effects, which have been heretofore neglected in the interpretation of OMEGA neutron spectra. At the backscatter edge, neglecting rescattering on OMEGA can lead to a ~10 to 20% reduction of the apparent areal density and therefore must be included in the analysis. The low ρR s on OMEGA also mean that backgrounds from non-target physics effects, such as scattering in the target chamber or slow scintillator decays, can significantly alter the measured signal. Here, we discuss how the Monte Carlo neutron spectrum postprocessor IRIS is used to include second-order scattering effects in the interpretation of the scattered neutron spectrum in OMEGA implosion experiments, and how dedicated implosion experiments are used to measure nTOF backgrounds in order to infer backscattered areal densities on OMEGA.
This report documents an evaluation of 240 Pu prompt fission neutron spectra (PFNS) including Chi-Nu experimental data. This work is a FY2025 Q4 NCSP (Nuclear Criticality Safety Program) milestone and named a “strategic priority”. This evaluation is new; it differs substantially from the most recent evaluation included in the ENDF/B library, which was for ENDF/B-VII.1 and then carried over unchanged to ENDF/B-VIII.1. The key difference between ENDF/B-VIII.1 and the new evaluation is that we have, for the first time, realistic experimental 240 Pu PFNS covering a broad incident and outgoing neutron energy range.
A new prompt fission neutron spectra (PFNS) measurement in the 238 U(n,f) reaction was performed at LANSCE/WNR facility. Evaluated data show discrepancies on the low (below 1 MeV) and high (above 5 MeV) energy parts in the PFNS for different major and minor actinides. The goal is to improve these measurements in a wide range of incident energy. The energy of the incoming neutron, inducing the fission, and the prompt neutron energies, are measured by time-of-flight method. A dedicated fission chamber was developed, in order to improve alpha-fission discrimination, timing resolution, actinide mass, and to reduce the amount of neutron scattering. To detect prompt neutrons, the 54 Chi-Nu scintillator cells array were surrounding the fission chamber. High statistics were recorded during this experiment, allowing a precise study of PFNS behavior as a function of incident neutron energy, from 1 MeV to 200 MeV. In conclusion, this experiment also showed that all the new tools developed to improve PFNS measurements are performing. Therefore, measurements of PFNS with others actinides such as 239 Pu are planned.
Unrecognized sources of uncertainty (USU) can bias the reported mean and/or covariance of experimental nuclear data. These biases, in turn, can propagate through evaluated nuclear data to application simulations or may poorly inform nuclear theory that is fitted to the experimental data. Such unknown sources of bias must be tied to the inherent physical constituents of the measurements such as the characteristics of a detector response or a background reduction technique. Here, in this article, a sparse Bayesian learning model is used to support experts in their efforts to identify and characterize USU in experimental prompt fission neutron spectra (PFNS) for spontaneous fissioning of 252 Cf by linking observed biases to features of the measurement system. Three different bias components were found. The first acts as a verification case for the algorithm as it identifies a bias coming from a well-known source related to the use of 6 Li in the neutron detection system. The second two cases demonstrate how this method can benefit the evaluation of experimental nuclear data by identifying, quantifying, and relating unknown biases to potential causes.
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 252 Cf, 235, 238 U, and 239 Pu PFNS, and enhanced by expertise from experimenters contributing to these PFNS templates.
Inelastic neutron scattering (INS) is uniquely sensitive to hydrogen due to its comparatively large thermal neutron scattering cross-section (82 b). Consequently, the inclusion of water in real samples presents significant challenges to INS data analysis due directly to the scattering strength of hydrogen. Here, we investigate uranyl fluoride (UO 2 F 2 ) with inelastic neutron scattering. UO 2 F 2 is the hydrolysis product of uranium hexafluoride (UF 6 ), and is a hygroscopic, uranyl-ion containing particulate. Raman spectral signatures are commonly used for inferential understanding of the chemical environment for the uranyl ion in UO 2 F 2 , but no direct measurement of the influence of absorbed water molecules on the overall lattice dynamics has been performed until now. To deconvolute the influence of waters on the observed INS spectra, we use density functional theory with full spectral modeling to separate lattice motion from water coupling. In particular, we present a careful and novel analysis of the Q-dependent Debye–Waller factor, allowing us to separate spectral contributions by mass, which reveals preferential water coupling to the uranyl stretching vibrations. Coupled with the detailed partial phonon densities of states calculated via DFT, we infer the probable adsorption locations of interlayer waters. We explain that a common spectral feature in Raman spectra of uranyl fluoride originates from the interaction of water molecules with the uranyl ion based on this analysis. In conclusion, the Debye–Waller analysis is applicable to all INS spectra and could be used to identify light element contributions in other systems.
We present the vibrational spectra of polyacrylonitrile-based carbon fibers collected using inelastic neutron scattering. We ascertain the behavior of a broad range of vibrational spectra that are optically silent, and demonstrate a direct connection between these modes and thermomechanical properties of the fibers. We show directionally dependent coupling of hydrogen in the carbon fiber matrix, which is directly linked to mechanical properties. Further, we show hydrogen preferentially couples to the midband of the vibrational spectrum, and that there are higher overall mode populations in the traditional Raman D–G intervalley region, suggesting involvement of these modes in tensile strength reduction and transport properties.
Retrospective characterization of a (30 MeV D, Be) neutron source was performed employing multi-foil activation and STAYSL-PNNL. Experimental reaction rates were calculated from gamma spectroscopy measurements of irradiated foils and MCNP provided the guess spectrum. Adjusted spectra were evaluated through activation calculations for a stainless-steel target using FISPACT-II. Adjusted spectra showed limited dependence on the dosimetry reactions and provided minor improvements in activation calculations. Omitting reflected neutrons in the guess spectrum generated poor activation results and the limited number of dosimetry reactions introduced doubt in the adjusted spectra. Furthermore, a dedicated neutron spectrometry experiment and a more detailed simulation is required.
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A method for estimating covariance matrices which capture the uncertainties in calculated reactor spectra has been developed. This method is based on perturbing the parameters of a physics-based analytic model fitted to a calculated spectrum. The covariance of the perturbed analytic spectra imposes energy-dependent correlations due to the physics of the neutron processes in the reactor, i.e., a fission component, a 1/E down-scatting component, and a thermal Maxwellian component. An analytic model is developed which is shown to produce good fits to several reactor environments. The covariance matrices produced via this method are then used as the prior spectrum in STAYSL least squares spectrum adjustment where it is combined with integral metrics, such as activation measurements, to produce a high-fidelity neutron spectrum characterization. It was concluded that the methodology showed agreeable results for the ACRR free-field spectrum adjustment in STAYSL resulting in a 𝜒 2 value of 2.21 (per degree of freedom), but further work is needed to describe scattering and interface regions.
Uranium tetrafluoride hydrate (UFH) is formed by immersing anhydrous UF4 under water for 12 h. UFH is therefore clearly a chemical species of environmental concern, as anhydrous UF4 is an intermediate uranium form in the nuclear fuel cycle. We use inelastic neutron scattering (INS) to probe the full vibrational spectra of UFH and its deuterated analogue in an effort to improve the fundamental understanding of its vibrational spectra. Coupled with density functional theory (DFT) calculations, the first for this compound, and full spectral modeling, we generate the complete vibrational spectra of UFH and compare them to prior optical spectroscopic results. In particular, the combination of DFT with INS allows us to identify multiple distinct chemical environments in the water bending and OH stretching regions. Whereas the water molecules directly bound to the U atoms execute OH stretching around 3600 cm –1 , a second class of H-bonded waters vibrate below 3000 cm –1 , an indicator of strong H bonding. In addition, a class of librational water modes are observed between 400 and 900 cm–1, which themselves can be separated in energy according to their chemical environments. Furthermore, measurements presented herein directly assist in the assignment of certain spectral features in the infrared spectrum and will inform future investigations of UFH for environmental or forensics purposes.
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.
A fused silica Cherenkov radiator has been utilized at the National Ignition Facility to provide a new high precision measurement of the time-of-flight spectrum of 14.1 MeV DT fusion neutrons. This detector allows a high precision (<30 ps) co-registered measurement of both a thresholded γ-ray and a neutron spectrum on a single record. Other approaches typically require γ and neutron signals to be co-registered via other diagnostics and/or dedicated timing experiments. Analysis of the co-registered γ and neutron signals allows precise extraction of the mean neutron energy and bulk hot-spot velocity, both of which were not possible with prior scintillator technologies. Initial measurements demonstrate the feasibility of this measurement and indicate that combined detection of neutrons and γ-rays on multiple lines-of-sight should enable the bulk vector velocity of the implosion hot-spot to be determined to ≈5 km/s and reduced uncertainty in the spectral width ≈0.1 keV.