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Event-by-event neutron–photon multiplicity correlations in 252Cf(sf)

Excited nuclear fragments are emitted during nuclear fission. The de-excitation of these fission fragments takes place as sequential emission of neutrons followed by photons. A correlation between neutron and photon multiplicities accompanying fission is thus expected. Fission event generators based on established statistical nuclear physics models predict a negative event-by-event correlation in neutron-photon multiplicity. A survey of published experimental results of an event-by-event covariance between the neutron - photon multiplicities emitted following the spontaneous fission of 252 Cf is presented. Analytic unfolding expressions are developed in this work to determine the bias introduced by background sources, particle misclassification, pulse pileup, and inelastic photon production. The published experimental data are re-analyzed using these unfolding techniques and are found to be in qualitative agreement with the predictions of model-based calculations. Finally, in particular, we have concluded that there exists a significant event-by-event neutron-photon emission competition following the spontaneous fission of 252 Cf.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

(U) Release of SOURCES4D Featuring Sensitivity Capabilities

SOURCES is a code for computing neutron source rates and spectra from spontaneous fission (including delayed neutrons) and (α,n) reactions. The first release since 2002, SOURCES4D, is now available. The main updates include new output that allows the user to calculate, in post-processing, first and second derivatives of the (α,n) source rate density and spectrum with respect to nuclide densities in a homogeneous material and first derivatives of the (α,n) source rate density and spectrum with respect to nuclide stopping powers and (α,n) cross sections (nuclear data). The value of π was made more accurate in order to eliminate negative spontaneous-fission sources. Otherwise, SOURCES4D has made no changes to the physics or data of neutron source calculations used in SOURCES4C. First and second derivatives are calculated in an example problem.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Modeling Kilonova Light Curves: Dependence on Nuclear Inputs

The mergers of binary neutron stars, as well as black hole–neutron star systems, are expected to produce an electromagnetic counterpart that can be analyzed to infer the element synthesis that occurred in these events. We investigate one source of uncertainties pertinent to lanthanide-rich outflows: the nuclear inputs to rapid neutron capture nucleosynthesis calculations. We begin by examining 32 different combinations of nuclear inputs: eight mass models, two types of spontaneous fission rates, and two types of fission daughter product distributions. We find that such nuclear physics uncertainties typically generate at least one order of magnitude uncertainty in key quantities such as the nuclear heating (one and a half orders of magnitude at 1 day post-merger), the bolometric luminosity (one order of magnitude at 5 days post-merger), and the inferred mass of material from the bolometric luminosity (factor of 8 when considering the 8–10 day region). Since particular nuclear processes are critical for determining the electromagnetic signal, we provide tables of key nuclei undergoing β-decay, α-decay, and spontaneous fission important for heating at different times, identifying decays that are common among the many nuclear input combinations.

79 ASTRONOMY AND ASTROPHYSICS↗

Mineral detection of neutrinos and dark matter. A whitepaper

Minerals are solid state nuclear track detectors — nuclear recoils in a mineral leave latent damage to the crystal structure. Depending on the mineral and its temperature, the damage features are retained in the material from minutes (in low-melting point materials such as salts at a few hundred °C) to timescales much larger than the 4.5 Gyr-age of the Solar System (in refractory materials at room temperature). The damage features from the O (50) MeV fission fragments left by spontaneous fission of 238U and other heavy unstable isotopes have long been used for fission track dating of geological samples. Laboratory studies have demonstrated the readout of defects caused by nuclear recoils with energies as small as O (1) keV. This whitepaper discusses a wide range of possible applications of minerals as detectors for E R ≳ O (1) keV nuclear recoils: Using natural minerals, one could use the damage features accumulated over O (10) Myr–O (1) Gyr to measure astrophysical neutrino fluxes (from the Sun, supernovae, or cosmic rays interacting with the atmosphere) as well as search for Dark Matter. Using signals accumulated over months to few-years timescales in laboratory-manufactured minerals, one could measure reactor neutrinos or use them as Dark Matter detectors, potentially with directional sensitivity. Research groups in Europe, Asia, and America have started developing microscopy techniques to read out the O (1)–O (100) damage features in crystals left by O (0.1)–O (100) keV nuclear recoils. We report on the status and plans of these programs. Furthermore, the research program towards the realization of such detectors is highly interdisciplinary, combining geoscience, material science, applied and fundamental physics with techniques from quantum information and Artificial Intelligence.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

High Resolution Fission Fragment Spectroscopy with Superconducting Microcalorimeters

Sub-1 AMU mass determination is important for determining fission yields and neutron multiplicity, which are necessary inputs for fission models. Fission models can improve spent nuclear waste stream analysis and nuclear fuel burnup determination. Here, to achieve this goal, we have used superconducting microcalorimeter detectors to directly measure the energy of fission fragments from the spontaneous fission of 252 Cf. With a fiber coupled LED pulser setup we demonstrate that we can reach a relative energy resolution of 0.1% and better for photon pulses with energies above 60 MeV. This instrument, in conjunction with time-of-flight (TOF) measurement, would allow for sub-1 atomic mass unit (AMU) mass determination of fission fragments in a future beamline application.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Machine learning-assisted identification of potential sources of bias in measurements of prompt-fission neutron spectra

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.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Structure of even-even Sr isotopes with 50 ≤ N ≤ 58 neutrons

Excited levels in Sr 90 , Sr 92 , Sr 94 , and Sr 96 nuclei were reinvestigated using high-statistics multiple- γ coincidence data from neutron-induced fission of U 235 and spontaneous fission of Cf 252 , measured using Exogam at Institut Laue Langevin and Gammasphere arrays, respectively. The experimental goal was the search for new excited levels and firm spin-parity assignments to known levels. A total of 23 new levels with 30 new or corrected decays and 39 new or improved spin-parity assignments were obtained in the four nuclei. Negative-parity structures on top of 3 - excitation were firmly identified and extended to higher spins. New positive-parity structures in Sr 94 and Sr 96 were observed with 3 + excitations characteristic of γ collectivity. The 277.7-keV, E 2 decay from the 1507.0-keV level to the second 0 + level in Sr 96 , found in this paper, completes the coexisting deformed band in this nucleus. To learn about the microscopic structure of levels in the Sr 88 - 96 nuclei, we performed large-scale shell-model calculations. The calculations compared to the experiment, helped the discussion of the evolution of collectivity in strontium isotopes, highlighting the important role of various single-particle excitations in phase transitions and shape coexistence in the region. The special role of the neutron 9 / 2 + [ 404 ] extruder as a catalyst of the deformation change in the region is highlighted.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Measurement of fragment-correlated γ-ray emission from 252 Cf(sf)

This paper presents recent experimental results on the yield of prompt fission γ rays from the spontaneous fission of 252 Cf. We use an ionization chamber to tag fission events and measure the masses and kinetic energies of the fission fragments and trans-stilbene organic scintillators to measure the neutrons and γ rays emitted by the fission fragments. The combination of the ionization chamber and trans-stilbene scintillators allows us to determine the properties of neutrons and γ rays in coincidence with the fragments. The yield of γ rays is known to be influenced by the angular momenta (AM) of the fission fragments. We present experimental evidence indicating that the total γ-ray multiplicity, i.e., the sum of both fragments' emission, saturates at sufficiently high internal fragment excitation energies. We also observe distinct behaviors for the yield of γ rays from the light and heavy fragments, which for certain mass and total kinetic energy (TKE) regions are weakly or anticorrelated, indicating the presence of complex AM generation modes. We also observed a mass- and TKE-dependent anisotropy of the γ rays, which challenges and expands on the conventional notion that the fragments' AM are always aligned perpendicularly to the fission axis. Furthermore, the dependence of the anisotropy on mass and TKE indicates a dependence of these properties on the specific fission channels, thus providing an insight into the deformations and dynamics in fission and their connection with experimentally observable quantities.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Building surrogate models of nuclear density functional theory with Gaussian processes and autoencoders

From the lightest Hydrogen isotopes up to the recently synthesized Oganesson (Z = 118), it is estimated that as many as about 8,000 atomic nuclei could exist in nature. Most of these nuclei are too short-lived to be occurring on Earth, but they play an essential role in astrophysical events such as supernova explosions or neutron star mergers that are presumed to be at the origin of most heavy elements in the Universe. Understanding the structure, reactions, and decays of nuclei across the entire chart of nuclides is an enormous challenge because of the experimental difficulties in measuring properties of interest in such fleeting objects and the theoretical and computational issues of simulating strongly-interacting quantum many-body systems. Nuclear density functional theory (DFT) is a fully microscopic theoretical framework which has the potential of providing such a quantitatively accurate description of nuclear properties for every nucleus in the chart of nuclides. Thanks to high-performance computing facilities, it has already been successfully applied to predict nuclear masses, global patterns of radioactive decay like β or γ decay, and several aspects of the nuclear fission process such as, e.g., spontaneous fission half-lives. Yet, predictive simulations of nuclear spectroscopy—the low-lying excited states and transitions between them—or of nuclear fission, or the quantification of theoretical uncertainties and their propagation to basic or applied nuclear science applications, would require several orders of magnitude more calculations than currently possible. However, most of this computational effort would be spent into generating a suitable basis of DFT wavefunctions. Such a task could potentially be considerably accelerated by borrowing tools from the field of machine learning and artificial intelligence. In this paper, we review different approaches to applying supervised and unsupervised learning techniques to nuclear DFT.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Characterizing Shielded Special Nuclear Material by Neutron Capture Gamma-Ray Multiplicity Counting

We present a new neutron multiplicity counting analysis and measurement method for neutron-shielded fissile material using neutron-capture gamma rays. Neutrons absorbed in shielding produce characteristic gamma rays that preserve the otherwise lost neutron multiplicity signature. Neutron multiplicity counting provides estimates of fission parameters, such as neutron leakage multiplication, spontaneous fissioner (e.g. Pu-240) mass, and (α,n) ratio. Standard neutron multiplicity counting can incorporate the new neutron-capture gamma-ray multiplicity counting technique to characterize previously degenerate or intractable source configurations by maximizing the multiplicity signature. The new method decouples neutron source-detector interferences, such as reflection and thermalization time in the detector, that could improve measurements of the mean neutron lifetime. We also develop a detector prototype for the multiplicity counting of neutron-capture gamma rays and present detector design considerations, such as detection material and shielding, to optimize the detection of the 2.2 MeV hydrogen capture gamma ray. We simulate the prototype neutron- capture gamma-ray multiplicity counter against the BeRP ball in polyethylene shells to inform future measurements.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Competition between mass-symmetric and asymmetric fission modes in 258 Md produced in the 4 He+ 254 Es reaction

Earlier studies of spontaneous fission of heavy actinides found that the fission-fragment mass distribution suddenly changes from predominantly asymmetric to symmetric, when the mass number of the fissioning nucleus becomes larger than A c = 257. We have measured for the first time fission-fragment mass and totalkinetic-energy (TKE) distributions of the excited compound nucleus 258 Md∗ (Z = 101), populated in the reaction 4 He + 254 Es, using the rare radioactive target isotope 254 Es with a short half-life, T1/2 = 275.7 d. The fission of 258 Md∗ can be interpreted as involving three fission modes: one mass-asymmetric and two mass-symmetric fission modes, the latter two are manifested by different TKE values. In this assumption, symmetric and asymmetric fission modes have nearly similar yields at the excitation energy of 15.0 MeV. The spectrum of 18.0 MeV can be explained as due to the increase of asymmetric fission mode.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Excited levels in odd-A silver isotopes populated rn fission of {sup 252}Cf

Excited levels in 111−121 Ag , odd-𝐴 isotopes populated following spontaneous fission of 252 Cf have been studied using high-fold 𝛾 coincidences measured with Gammasphere array of Compton-suppressed Ge spectrometers at Argonne National Laboratory. The experimental information on these nuclei reported before has been corrected and extended. In the work we discuss the evolution of triaxiality in odd-Ag nuclei. Relative positions of the 𝜋⁢𝑝1/2 and 𝜋⁢𝑔9/2 shells defining the 𝑍=40 gap when approaching the 𝑁=82 closure, the 𝜋⁢1/2+⁢[431] intruder bands, the three-quasiparticle configurations, and the so called 𝑗−1 anomaly in odd-Ag nuclei are also discussed.

Urban, W.↗

Microscopic evidence for scission neutrons

We discuss the neck rupture stage of fission and the emission of particles afterwards, two extremely rapid and highly non-equilibrium processes. Currently, the neck rupture cannot be directly probed by experiment, highlighting the importance of reliable theoretical predictions for this stage of fission. Time-dependent density functional theory (TDDFT) is used to simulate the spontaneous fission of 252 Cf. In conjunction with statistical models, inputs from microscopic calculations can be used to make predictions for prompt neutron and gamma emission spectra, quantities which can be experimentally measured. Here we characterize the scission mechanism within TDDFT and estimate the number of scission neutrons and their kinetic energies.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Shape evolution in neutron-rich odd-even 105–109 Nb isotopes

Background: Neutron-rich nuclei around 𝑍 ≈ 40 are well known for exhibiting multiple shape transitions. Here, this region shows one of the sharpest shape transitions in the nuclear chart, evolving from a spherical vibrator at 𝑁 = 58 to a strongly deformed prolate shape at 𝑁 = 60. The largest deformations are observed for 38 Sr and 40 Zr . This abrupt shape transition disappears at 𝑍 = 36 and below, where a shape transition from spherical to oblate nuclei is predicted. On the other hand, for 𝑍 ≥ 42 and 𝑁 ≥ 60, the shape is known to evolve from axial to triaxial. While the even-𝑍 nuclei in this region have already been extensively studied, new insights can be gained from the studies of odd-𝑍 isotopes for a better understanding of the underlying mechanisms driving these phenomena. Purpose: The 41 Nb nuclei lie at the boundary between axially deformed Zr and triaxially deformed Mo nuclei. This work investigates the nuclear structure of very neutron-rich Nb nuclei up to 𝑁 = 68. The goal is to understand how the nuclear shape evolves as a function of isospin in this isotopic chain and provide new insights into the emergence of triaxial deformation. Methods: The structure of the neutron-rich Nb isotopes was investigated using state-of-the-art high-resolution 𝛾-ray spectroscopy of fission fragments produced via two different fission reactions. The use of 9 Be ⁢( 238 U, 𝑓) inverse kinematics, with a detection system comprising AGATA, EXOGAM, and VAMOS++, enabled the measurement of prompt and delayed 𝛾 rays from isotopically identified fission fragments, and 𝛾−𝛾−𝛾−𝛾 highfold data were obtained from a spontaneous fission source of 252 Cf using the Gammasphere array. Results: The level scheme of 105 Nb has been significantly extended, with the addition of two negative-parity bands observed for the first time. A new level scheme is proposed for 107 Nb, which is not in agreement with an earlier measurement, and new levels and transitions have been added to the very neutron-rich 109 Nb. The degree of triaxiality of the new bands is discussed on the basis of signature splitting analysis. The recently reported level scheme of 99 Nb has been revised. Conclusions: This systematic study on the Nb isotopic chain, compared to Zr and Mo, indicates that while the ground-state band exhibits a triaxial deformation, attributed to a proton hole coupled to a triaxially deformed Mo core, the negative-parity bands, based on isomeric bandheads, display an axially symmetric deformed structure, similar to that observed in the Zr isotopes, revealing the existence of a shape coexistence in the neutron-rich Nb nuclei.

Abushawish, M. [Université Claude-Bernard Lyon 1 (↗

Microscopic Evidence for Scission Neutrons

We discuss the neck rupture stage of fission and the emission of particles afterwards, two extremely rapid and highly non-equilibrium processes. Currently, the neck rupture cannot be directly probed by experiment, highlighting the importance of reliable theoretical predictions for this stage of fission. Time-dependent density functional theory (TDDFT) is used to simulate the spontaneous fission of 252 Cf. In conjunction with statistical models, inputs from microscopic calculations can be used to make predictions for prompt neutron and gamma emission spectra, quantities which can be experimentally measured. Here we characterize the scission mechanism within TDDFT and estimate the number of scission neutrons and their kinetic energies.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Measurement of the 252 Cf ⁢(sf) prompt fission neutron spectrum utilizing 12 C ⁡(𝑛, 𝑛) and 9 Be ⁢(𝑛, 𝑛) neutron scattering reference measurements

The 252 Cf spontaneous fission (sf), prompt fission neutron spectrum (PFNS) is a fundamental quantity for nuclear physics measurements of neutron-emitting reactions. This energy distribution of neutrons emitted from fission has been considered a neutron data standard for decades and has been utilized as a reference for neutron detection efficiency, validation of Monte Carlo simulations, benchmarking of dosimetry standards, and more. A significant portion of the global collection of nuclear data on neutron-induced reactions is correlated with the 252 Cf ⁢(sf) PFNS. Despite the reliance on this quantity by the nuclear physics community, the historical collection of 252 Cf PFNS measurements display systematic disagreements that are not understood or easily explained. These experimental discrepancies could potentially bias the 252 Cf PFNS Standard evaluation. On top of this, these past experiments frequently employed correlated experimental measurement or analysis methods. The artificial intelligence (AI)/machine learning (ML)-informed californium chi-nuclear data experiment (AIACHNE) project was formed to (a) investigate these discrepancies utilizing AI/ML methods to identify outlying regions of literature data, assign these regions to features of the experiment itself, and perform an improved evaluation of the 252 Cf PFNS and (b) perform a new experimental measurement of this quantity designed to improve upon the existing literature database. Here, in this work, we report on the AIACHNE 252 Cf PFNS experiment utilizing a new analysis method uncorrelated with all previous measurements: neutron efficiency determinations based on elastic neutron scattering on 12 C and 9 Be . This new method provides an independent test of the existing literature data and evaluation of the 252 Cf ⁢(sf) PFNS. The method is described with detailed covariance quantification procedures, as well as a direct discussion of the sources of uncertainty described as requirements in the “Templates” series of papers. The 252 Cf ⁢(sf) PFNS reported in this work agrees well with the overall shape of the existing standard PFNS evaluation as well as many literature measurements, thus verifying the current evaluation utilizing new techniques. However, the results suggest that there are deficiencies in the angle-differential 12 C and 9 Be ⁢(𝑛, 𝑛) evaluated nuclear data, which produce unphysical structures in the reported result. While these structures are relatively minor, they become obvious because of the high statistical precision of the data and the expected smooth continuity of the 252 Cf ⁢(sf) PFNS.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Errors introduced in fission neutron spectrum measurements using a single reference

Measurements of physical quantities are often made relative to a reference quantity, simplifying the interpretation of the measurement and its uncertainties. However, if applied without careful considerations, this technique can carry with it a significant and complex systematic error that is usually ignored. For example, measurements of continuous neutron spectra relative to a reference spectrum yield a result that does not properly include the important effects of neutron scattering in the experimental environment. These effects act to distort the measured spectrum shape and create notable errors in spectrum-integrated quantities. While this effect is one of a series of known potential sources of systematic error including, but not limited to target impurities, angular distributions, incident beam flux, and others, the error introduced from differences in environmental scattering effects between the reference and desired spectra are frequently overlooked. In this work, we demonstrate the origin of this error using simulated data corresponding to measurements of the neutron-induced prompt fission neutron spectra of 233 U, 235 U, 238 U, and 239 Pu as well as the spontaneous fission neutron spectrum of 252 Cf. Errors in the spectrum shape can be as high as 10%–15% depending on the combination of incident and outgoing neutron energy. The spectrum integral and average spectrum energy also contain errors that change with incident neutron energy and can be as high as ~2%. Although this study is based on simulated data, we also show a method for proving that this error exists in an experimental data set and we show a correction that can be applied to results of this type to obtain a more accurate result, thereby largely removing systematic errors from environmental scattering effects. The potential for these kinds of errors should be considered in measurements producing continuous neutron spectra.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Instrumentation for correlated prompt n – γ emission studies in coincidence with fission fragments

Recent theoretical and experimental results have brought renewed interest and focus on the topic of fission fragment angular momentum. Measurements of neutrons and rays in coincidence with fission fragments remain the most valuable tool in the exploration of fission physics. To achieve these scientific goals, we have developed a system that combines a state-of-the-art fission fragment detector and n – γ radiation detectors. A new twin Frisch-gridded ionization chamber has been designed and constructed for use with a spontaneous fission source and an array of forty trans-stilbene organic scintillators (FS-3) at Argonne National Laboratory. The new ionization chamber design we present in this work aims at minimizing particle attenuation in the chamber walls, and provides a compact apparatus that can be fit inside existing experimental systems. The ionization chamber is capable of measuring fission fragment masses and kinetic energies, whereas the FS-3 provides neutron and γ-ray multiplicities and spectra. Here, the details of both detector assemblies are presented along with the first experimental results of this setup. Planned event-by-event analysis and future experiments are briefly discussed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗