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Erratum: Monoenergetic photon-induced fission cross-section ratio measurements for U 235 , U 238 , and Pu 239 from 9.0 to 17.0 MeV

In this erratum we report a correction to the previously published photofission cross-section ratio data. The actinide fission-chamber foils utilized in this work were extensively characterized during a new campaign using α- and γ-ray spectroscopy, and 2π alpha counting. These three techniques agreed, resulting in an improved accuracy of the fission-chamber foil masses used in the original experiment. The foil masses measured by α spectroscopy are detailed in Table I. All foils were counted on the same α spectrometer, using an identical geometry, which reduces the systematic uncertainty in the calculated mass ratios since the α spectrometer efficiency cancels out in the ratio. This results in a relative uncertainty on the mass ratio of 1.0% for 235 U/ 238 U, 0.62% for 239 Pu/ 235 U, and 1.1% for 239 Pu/ 238 U. The published cross-section ratio data are re-calculated to reflect the updated target masses and uncertainties. The new mass values cause a 2.40% decrease for the σ( 235 U(γ, f)/ 238 U(γ, f)) ratio, a 5.10% decrease for the σ( 235 U(γ, f)/ 239 Pu(γ, f)) ratio, and a 2.77% decrease for the σ( 238 U(γ, f)/ 239 Pu(γ, f)) ratio. The updated cross-section ratios are presented in Tables II, III, and IV, which are corrected versions of Tables III, IV, and V in Ref. [1]

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Revision of forensics-relevant nuclear data in Sb 127 β decay

With a half-life of 3.85(5) d, the fission product 127 Sb is potentially useful for the characterization of fallout debris that would be collected for forensic analysis following a hypothetical nuclear event. The β decay of 127 Sb has many characteristic $\gamma$-ray lines, however, the majority of decay strength is concentrated in the three strongest lines near 686, 473, and 784 keV, based on low-precision spectroscopic measurements from decades ago. In a new measurement of 127 Sb β decay, obtained from radiochemical separations of U photofission products, we show that the energies of the 686 and 784 lines are actually shifted lower by 0.8 and 1.1 keV, respectively. Such large discrepancies in the nuclear data inhibit accurate isotopic analyses and have important implications, for example, on the assessment of fission debris that might be collected in the days following a nuclear event. Therefore, a new evaluation of 127 Sb β decay and appropriate revision to the various nuclear databases are warranted. This work reports a new set of $\gamma$-ray energies and relative intensities corresponding to 127 Sb decay.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Fission Gamma-Ray Spectra Relevant to Post-Detonation Debris Analysis

A terrorist-generated nuclear attack would invoke unprecedented pressure for a rapid and accurate nuclear forensics characterization of the event. In-situ fission product gamma-ray spectroscopy offers the potential for a significant reduction in analysis time while still providing high fidelity identification of the primary composition of the detonated device. The in-situ spectroscopic approach we are proposing can rapidly identify the species that underwent fission as well as the fission-inducing neutron energy spectrum. To demonstrate this goal, we have used the gammaray history from our previously obtained LLNL-LANL-TUNL fission product-yield (FPY) data to provide insights for post-detonation debris analysis. The proposed method relies on the ratio of photopeak areas for selected gamma-rays representing the FPYs of sixteen fission products generated using mono-energetic neutrons at energies between 0.5 MeV to 14.8 MeV on highlyenriched 239 Pu, 235 U, and 238 U sealed targets. In addition to the fission product ratio measurements we have applied a new regression analysis based on our experimental FPY data and validated the approach using relevant Godiva FPY data and (surrogate) photofission product yields of 240 Pu. The main advantage of the regression analysis is that it investigates the FPY data set as a whole, rather than focusing on individual FPY ratios.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Fission with Exotic Nuclei (Abbreviated Report)

Nuclear fission is a key mechanism involved in the synthesis of heavy elements in the Cosmos and is the primary explanation for the stability of superheavy elements. Nevertheless, our knowledge of fission remains extremely fragmented. Most experiments have been conducted only on a tiny number of stable actinide nuclei and are often incomplete, leading to gaps in our basic understanding of the process. For many radioactive isotopes, basic fission data such as the charge or mass distribution of the fragments is unknown. These gaps cannot always be filled by simulation alone. Common fission models contain too many free parameters and lack predictive power. In contrast, the fundamental theory of fission under development at LLNL is much more predictive, but its current computational cost is too high to be used extensively for data evaluations. A unique window of opportunity to resolve these limitations has recently opened: the U.S. nuclear science community is ramping up major experimental programs at the Facility for Rare Isotope Beams (FRIB, the DOE flagship facility in low-energy nuclear science), and techniques from machine learning have shown great potential to simplify the use of a fundamental, quantum-mechanical theory of fission. This project has two components. On the experimental side, we acquired and deployed at the HIGS facility a new dual Frisch-Grid ionization chamber to measure correlated fragment-mass, kinetic energy, and angular distributions of fission fragments from induced fission. This new device was used to perform measurements of charge, mass and total kinetic energy of fission fragments in the photofission of 238 U and eight gamma-ray beam energies between 6.2 and 13 MeV, which allowed extracting high-precision independent yields for this reaction. The device was also used to perform measurements of the same quantities in the neutron-induced fission of 234 U with monoenergetic beams of energy between 5 and 8 MeV. In parallel, we collaborated with a team at Commissariat à l’énergie atomique et aux énergies alternatives (CEA) to perform a series of measurements of fission yields in inverse kinematics for the two isotopes of 236 U and 240 Pu. The experiment took place at the Grand Accélérateur National d’Ions Lourds in France in June 2023. The deployment of the VAMOS spectrometer with a new array called PISTA allowed determining the excitation energy of the fissioning system within 1 Mega-electronvolts. The second component of the project involved using deep neural networks to build fast and reliable emulators of our current fission models. In an invited paper published in Frontier in Physics, we showed that autoencoders could successfully compress nuclear wavefunctions in nuclear density functional theory. We achieved a dimensionality reduction of the order of two orders of magnitude while keeping the error in the total energy to less than 0.01%. In a second paper submitted to Physical Review Letters in June 2023 with our collaborators at CEA, we showed that variational autoencoders can learn the collective degrees of freedom driving the fission process.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Cosmological constraints on the lifetime of massive particles

Particles with masses more than a few MeV, decaying into photons or electrons, can cause destruction by photofission of cosmologically produced light elements. A previous calculation of this effect is corrected and extended, and used to derive maximum lifetimes for massive neutrinos; these range from a few thousand seconds upward, depending on the particle mass. Some approximate expressions are given that enable lifetime limits to be obtained for other particles, with different masses and abundances, such as gravitinos. These limits are generally stronger than previously determined constraints, such as distortion of the microwave background by energetic photons.

Lindley, D.↗

Experimental Quantification of the Background Neutron Flux in the Advanced Test Reactor Fuel Storage Canal

The Advanced Test Reactor (ATR) at the Idaho National Laboratory (INL) is one of only a few high-power research reactors (HPRR) of its type in the world, with a variety of missions involving accelerated testing of nuclear fuel and other materials in a very high neutron flux (5.0x1014 n/cm2 -s) environment, medical and industrial isotope production, and other applications. It typically runs several cycles per year with lengths varying from 40-60 days depending on specific experimental requirements for each cycle. The highly radioactive used fuel elements that are discharged from the ATR after each cycle are stored in an adjacent canal (Figure 1) and can be used for as many as three cycles before being retired. The ATR canal features a gamma irradiation facility that has various uses. It is composed of a simple dry tube that extends down into one of the fuel storage rack positions. This tube is surrounded by used fuel elements that can be selected from the inventory to produce the desired gamma radiation level and, to some extent, spectrum within the dry tube. Typical gamma fields that can be produced in this manner can be as high as several megarads per hour. The gamma field within the dry tube is accompanied by a small background neutron flux, produced by photoneutron production in the small fraction of heavy water (D2O) that is naturally present in light water at a concentration of approximately 0.015% by weight, and by a very low level of photofission and spontaneous fission in the fuel elements. The measurement technique used is very sensitive and provided self-consistent results in terms of raw activation data quality. The background neutron fluxes in the gamma facility are very low, but still detectable. The total neutron flux in the energy region from 0.414 eV to 1 MeV and the thermal neutron flux (below 0.414 eV) were estimated from the activation measurements to be 1.0x104 and 2.0x102 n/cm2 -s, respectively. ncertainties of approximately an order of magnitude apply to both results. No neutrons above about 1 MeV were detected. The high uncertainties quoted here are primarily due to uncertainties in the a priori neutron fluxes computed by MCNP6 as well as uncertainties in the spectrum-averaged foil activation cross sections used in the few-group least-squares flux adjustment procedure that was applied. Detailed analyses are currently underway with the aim of reducing these sources of uncertainty.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Fission product yield measurements using monoenergetic photon beams

High-accuracy fission product yield (FPY) data are needed to advance theoretical descriptions of the nuclear fission process, to improve the predictive power of phenomenological models, and for applications in nuclear energy, nuclear forensics, and homeland security. This paper reports the most complete data for measurements of product yields from photon-induced fission of 235 U, 238 U, and 239 Pu. Here, the measurements are performed using a monoenergetic photon beam of E γ = 13 MeV. More than 40 isotopes produced in fission were uniquely identified and their yield values were computed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Photonuclear reaction studies at HIγS: Developing the science of remote detection of nuclear materials

Development of gamma-ray beam interrogation technologies for remote detection of special nuclear materials and isotope analysis requires comprehensive databases of nuclear structure information and gamma-ray induced nuclear reaction observables. Relevant nuclear structure details include the energy, spin and parity of excited states that have significant probability for electromagnetic transition from the ground state, i.e, the angular momentum transferred in the reaction is Δl ≤ 2. This talk will report recent Nuclear Resonance Fluorescence (NRF) measurements to identify and characterize new low-spin states in actinide nuclei at energies from 1 to 4 MeV, which is the energy range most important for remote analysis methods. Here, these measurements are carried out using the nearly mono-energetic linearly polarized gamma-ray beam at the High Intensity Gamma-ray Source (HIγS) at the Triangle Universities Nuclear Laboratory. Also, studies of the (γ, n) reaction on a variety of nuclei with linearly polarized beams at HIγS indicate that this reaction might be used to discern between fissile and non-fissile materials. This work will be described. In addition, an overview will be given of a concept for a next generation laser Compton-backing scattering gamma-ray source to be implemented as an upgrade to increase the beam intensity at HIγS by more than an order of magnitude.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Delayed Gamma-Ray Spectroscopy for Non-Destructive Assay of Nuclear Materials

High-­energy, beta-delayed gamma-­ray spectroscopy is a potential, non-­destructive assay techniques for the independent verification of declared quantities of special nuclear materials at key stages of the fuel cycle and for directly assaying nuclear material inventories for spent fuel handling, interim storage, reprocessing facilities, repository sites, and final disposal. Other potential applications include determination of MOX fuel composition, characterization of nuclear waste packages, and challenges in homeland security and arms control verification. Experimental measurements were performed to evaluate fission fragment yields, to test methods for determining isotopic fractions, and to benchmark the modeling code package. Experimental measurement campaigns were carried out at the IAC using a photo-­neutron source and at OSU using a thermal neutron beam from the TRIGA reactor to characterize the emission of high-­energy delayed gamma rays from 235 U, 239 Pu, and 241 Pu targets following neutron induced fission. Data were collected for pure and combined targets for several irradiation/spectroscopy cycle times ranging from 10/10 seconds to 15/30 minutes.The delayed gamma-ray signature of 241 Pu, a significant fissile constituent in spent fuel, was measured and compared to 239 Pu. The 241 Pu/ 239 Pu ratios varied between 0.5 and 1.2 for ten prominent lines in the 2700-­3600 keV energy range. Such significant differences in relative peak intensities make it possible to determine relative fractions of these isotopes in a mixed sample. A method for determining fission product yields by fitting the energy and time dependence of the delayed gamma-­ray emission was developed and demonstrated on a limited 235 U data set. De-­convolution methods for determining fissile fractions were developed and tested on the experimental data. The use of high count-­rate LaBr 3 detectors was investigated as a potential alternative to HPGe detectors. Modeling capabilities were added to an existing framework and codes were adapted as needed for analyzing experiments and assessing application-­specific assay concepts. A de-­convolution analysis of the delayed gamma-­ray response spectra modeled for spent fuel assemblies was performed using the same method that was applied to the experimental spectra.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Active Interrogation of the Snyder Shells using a SEA-7 Betatron

The shielded highly enriched uranium (HEU) problem is one that still needs to be addressed. As a first step towards a solution, the Snyder shells (depleted uranium) were actively interrogated with a SEA-7 betatron in various configurations using an MC15 as a detector. These configurations include masses from 0.55 to 5.1 kg, as well as 5.1 kg in a steel container. A strong electromagnetic field (EMF) background was identified in previous work, but the results in this work show all configurations produce a signal well above the background. An initial simulation capability was developed that produces the expected flux profile from the SEA-7 betatron, but further work needs to be done to determine the magnitude of the flux via a combination of experiment and simulation validation. Depleted uranium generally produces more neutrons than HEU, so additional future work will need to include similar measurements of HEU to confirm similar performance of the technique. Additionally the EMF background needs to be better characterized as a function of distance and angle from the SEA-7 source and mitigation techniques explored.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗