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At least 613 records · Page 34

Gamma Rays from Kilonova: A Potential Probe of r-process Nucleosynthesis

The mergers of compact binaries with at least one neutron star component are the potential leading sites of the production and ejection of r-process elements. Discoveries of galactic binary pulsars, short gamma-ray bursts, and gravitational-wave detections have all been constraining the rate of these events, while the gravitational wave plus broadband electromagnetic coverage of binary neutron star merger (GW170817) has also placed constraints on the properties (mass and composition) of the merger ejecta. But uncertainties and ambiguities in modeling the optical and infrared emission make it difficult to definitively measure the distribution of heavy isotopes in these mergers. In contrast, gamma rays emitted in the decay of these neutron-rich ejecta may provide a more direct measurement of the yields. We calculate the gamma production in remnants of neutron star mergers, considering two epochs: a kilonova epoch, lasting about two weeks, and a much later epoch of tens and hundreds of thousands of years after the merger. For the kilonova epoch, when the expanding ejecta is still only partially transparent to gamma radiation, we use 3D radiative transport simulations to produce the spectra. Futhermore, we show that the gamma-ray spectra associated with beta- and alpha-decay provide a fingerprint of the ejecta properties and, for a sufficiently nearby remnant, may be detectable, even for old remnants. We compare our gamma spectra with the potential detection limits of next generation detectors, including the Lunar Occultation Explorer (LOX), the All-sky Medium Energy Gamma-ray Observatory (AMEGO), and the Compton Spectrometer and Imager (COSI). We show that fission models can be discriminated via the presence of short-lived fission fragments in the remnant spectra.

79 ASTRONOMY AND ASTROPHYSICS↗

Advanced Spacecraft Propulsion

This paper describes new propulsion concepts and research, and summarizes the goals and achievements of ongoing propulsion research.

fusion solar thermal beamed energy antimatter↗

Embedding Neural Thermal Scattering (NeTS) Modules in SERPENT for Higher Fidelity Advanced Reactor Analysis

When a neutron born in fission thermalizes to the order of $k$ $B$ $T$, it’s de-Broglie wavelength and energy approach the order of inter-atomic spacing and elementary lattice oscillations, respectively. $S$($a,β,t$) or the scattering law, uuantify these temperature-dependent crystallographic contributions to total cross section (or reaction rate). In a Monte Carlo analysis, cumulative distribution functions (CDFs) of $S$($a,β,t$) are loaded to memory from “A Compact ENDF” (ACE) files for stochastically selecting thermal scattered neutron trajectories. In this work, novel neural thermal scattering (NeTS) modules for $S$($a,β,t$) CDFs are designed, trained, serialized and embedded within SERPENT using Python’s limited C-API for on-the-fly deployment of crystalline graphite $S$($a,β,t$) sampling. Torchscript tracing and Numba just-in-time (JIT) compilation streamline neural inference on NVIDIA GPUs with CUDA libraries. Demonstrations of bare sphere thermalization of fast and thermal sources show excellent agreement between embedded NeTS in SERPENT and MCNP. With an explicit model of the reactor, NeTS can predict on-the-fly changes in TREAT neutron spectra as a function of local temperature, which can serve to improve transient and accident predictions in a multiphysics analysis framework. This framework can be further extended to account on-the-fly for changes in local graphitic microstructure to scattering cross sections, and outlines a novel coupling of modern machine learning with state-of-the-art reactor physics methods.

97 MATHEMATICS AND COMPUTING↗

Observation of new neutron-rich isotopes in the vicinity of Zr 110

Neutron-rich radioactive isotope (RI) beams in the vicinity of 110 Zr were produced using the in-flight fission of a 345-MeV/nucleon 238 U beam at the RIKEN Radioactive Isotope Beam Factory. Here, the RI beams were separated in flight by the large-acceptance two-stage fragment separator BigRIPS. Isotopes were clearly identified in a low-background particle-identification plot, which was obtained from the measurements of time of flight, magnetic rigidity, and energy loss using beam-line detectors placed in the BigRIPS separator and the ZeroDegree spectrometer. Nine new isotopes, 101 Br, 102 Kr, 105,106 Rb, 108 Sr, 110,111 Y, 114 Zr, and 117 Nb, are reported for the first time, with their measured production cross sections compared with the extrapolations of lighter isotopes down to the femtobarn regime.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Singlet fission and triplet pair recombination in bipentacenes with a twist

We investigate triplet pair dynamics in pentacene dimers that have varying degrees of coplanarity (pentacene–pentacene twist angle). The fine-tuning of the twist angle was achieved by alternating connectivity at the 1-position or 2-positions of pentacene. This mix-and-match connectivity leads to tunable twist angles between the two covalently linked pentacenes. These twisted dimers allow us to investigate the subtle effects that the dihedral angle between the covalently linked pentacenes imparts on singlet fission and triplet pair recombination dynamics. We observe that as the dihedral angle between the two bonded pentacenes is increased, the rates of singlet fission decrease, while the accompanying decrease in triplet recombination rates is stark. Temperature-dependent transient optical studies combined with theoretical calculations show that the triplet pair recombination proceeds primarily through a direct multiexciton internal conversion process. Calculations further show that the significant decrease in recombination rates can be directly attributed to a corresponding decrease in the magnitude of the nonadiabatic coupling between the singlet multiexcitonic state and the ground state. Furthermore, these results highlight the importance of the twist angle in designing systems that exhibit rapid singlet fission, while maintaining long triplet pair lifetimes in pentacene dimers.

14 SOLAR ENERGY↗

Development of bubble evolution model for new mechanistic transient fission gas release capability in BISON

This report summarizes efforts within NEAMS to investigate the mechanisms that govern fission gas behavior in UO 2 . In particular, the focus is on understanding how fission gas behavior causes transient fission gas release and fragmentation/pulverization of high burnup structure (HBS) in UO 2 . HBS forms in the periphery of the pellet where temperatures are relatively low. Previously, MD simulations were performed to determine the reaction energies for various Xe and U defects with bubbles, as a function of Xe to vacancy ratio or, equivalently, pressure. As had been shown in FY22, it was found that the unmodified version of the Simple Integrated Fission Gas Release and Swelling (SIFGRS) model within BISON greatly over-predicted the number gas atoms per vacancy in the bubbles in the outer rim of the pellet (a ratio of > 1 million). This was due to slow grain boundary vacancy diffusivity and not accounting for the pressure-dependent reaction energy for Xe interstitials with bubbles. The application of the pressure dependent reaction energies was able to restrict Xe to vacancy ratios to 2:1, which is far more realistic than those originally obtained from SIFGRS.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

New approach to precisely measure γ-ray intensities for long-lived fission products, with results for the decay of 95 Zr

For many fission products, the rays emitted following decay provide an easily-detectable signature that can be used to identify their quantities and distributions in a sample. As a result, γ-ray spectroscopy is often exploited to study fission-product yields, provided sufficiently accurate information on the γ-ray intensity is available. However, in many cases, the uncertainties in the existing nuclear data are large enough that they compromise the precision achievable for modern experiments and applications. To address this need, we have developed a new experimental method that is well suited to precisely measure absolute γ-ray intensities in the β decay of long-lived fission products. The approach involves the production of a radiopure sample by implantation of a mass-separated ion beam from the CAlifornium Rare Isotope Breeder Upgrade (CARIBU) facility on a thin carbon foil. The emitted β-decay radiation is detected with a 4π gas proportional counter and a meticulously efficiency-calibrated high-purity germanium (HPGe) detector. As a first measurement to demonstrate the approach, we studied the absolute γ-ray intensities of the strongest transitions following the β decay of 95 Zr and its decay-daughter 95 Nb, and determined them to fractional precisions of better than 1–2%. In addition, with a larger sample of activity produced through neutron irradiation of an isotopically-enriched Zr foil, we performed a high-precision measurement of the relative γ-ray intensities following the decay of 95 Zr with just the HPGe detector. Here, the sample-production method at CARIBU and the coincidence detection approach demonstrated here can be applied to study fission products with half-lives longer than a day, which includes isotopes important not only for nuclear-energy and national-security applications, but also for medical-isotope research and environmental monitoring.

4π↗

Skyrme–Hartree–Fock–Bogoliubov mass models on a 3D mesh: IIb. Fission properties of BSkG2

Large-scale models of nuclear structure are currently the only way to provide consistent datasets for the many properties of thousands of exotic nuclei that are required by nucleosynthesis simulations. In [W. Ryssens et al., Eur. Phys. J. A 58, 246 (2022)], we recently presented the new BSkG2 model based on an energy density functional of the Skyrme type. Relying on a flexible three-dimensional coordinate representation of the nucleus, the model takes into account both triaxial deformation and time-reversal symmetry breaking. BSkG2 achieves a state-of-the-art global description of nuclear ground state (g.s.) properties and reproduces in particular the known masses with a root-mean-square (rms) deviation of 678 keV. Moving beyond g.s. properties, the model also reproduces all empirical values for the primary and secondary barriers as well as isomer excitation energies of actinide nuclei with rms deviations below 500 keV, i.e. with unprecedented accuracy. Here we discuss in detail the extension of our framework to the calculation of the fission barriers of 45 actinide nuclei, including odd-mass and odd-odd systems. We focus in particular on the impact of symmetry breaking which is key to the accuracy of the model: we allow systematically for axial, reflection and time-reversal symmetry breaking. The effect of the latter on the fission properties of odd-mass and odd-odd nuclei is small, but we find that allowing for shapes with triaxial or octupole deformation, as well as shapes with both, is crucial to achieving this accuracy. Here, the numerical accuracy of our coordinate space approach, the variety of nuclear configurations explored and the simultaneous successful description of fission properties and known masses makes BSkG2 the tool of choice for the large-scale study of nuclear structure.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Fission-product decay studies with the FRIB Decay Station

The Facility for Rare Isotopes Beams (FRIB) will be the flagship facility in low-energy nuclear physics when it comes online in 2022. This U.S. Department of Energy Office of Science user facility will open up a multitude of new opportunities to study exotic nuclei and will lead to new discoveries in nuclear structure, nuclear astrophysics, fundamental symmetries, and isotopes of importance to nuclear applications. The b-decay properties of neutron-rich isotopes will be measured with the FRIB Decay Station, a sophisticated state-of-the-art modular multi-detector system envisioned to perform b, g, n, and charged-particle spectroscopy. In this feasibility study, we use nuclear decay data collected with the FRIB Decay Station precursor, the Beta-Counting Station, currently used at Michigan State University with a radioactive beam produced at the National Superconducting Cyclotron Laboratory to identify the FRIB Decay Station capabilities for future measurements of neutron-rich exotic nuclei at FRIB to help provide a path forward for future measurements of interest to the lab’s mission.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Identification and Quantification of Technetium Species in Hanford Waste Tank AN-102

Technetium-99 (Tc) generated from the fission of 235U and 239Pu in high yields is one of the most difficult contaminants to be addressed at the U.S. Department of Energy Hanford Site. In strongly alkaline solutions typifying Hanford tank waste, Tc exists as pertechnetate (TcO4-) (oxidation state VII) as well as in reduced forms (oxidation state < VII) collectively known as non-pertechnetate species. Designing strategies for effective Tc management, including separation and immobilization, necessitates understanding the molecular structure of the non- pertechnetate species and their identification in the actual tank waste samples, which would facilitate development of new treatment technologies effective for dissimilar Tc species. Toward this objective, a spectroscopic library of the Tc(I) [fac-Tc(CO)3]+ and Tc(IV, VII) compounds was generated using a range of techniques and applied to the characterization of the actual tank waste supernatant collected from the tank 241-AN-102 at Hanford, WA. A sample of the 241-AN-102 tank waste supernatant was processed to adjust Na concentration to about 5.6 M and remove 137Cs by spherical resorcinol-formaldehyde (sRF) ion exchange resin. Cesium-loaded sRF column was eluted with 0.5 M HNO3. As received AN-102, Cs-depleted AN-102 effluent, and sRF eluate fractions were comprehensively characterized for chemical composition and speciation of Tc using 99Tc nuclear magnetic resonance spectroscopy and X-ray absorption spectroscopy. It was demonstrated for the first time that non-pertechnetate Tc present in the 241-AN-102 tank waste is composed of several low-valent Tc species, including the Tc(I) [fac-Tc(CO)3]+ and Tc(IV) compounds. This is the second experimental observation of the [fac-Tc(CO)3]+ species in the Hanford tank waste and the first demonstration of multiple forms of non-pertechnetate species existing simultaneously in the waste, cumulatively highlighting their importance for the waste processing.

Low Activity Waste (LAW), High Level Waste, nuclea↗

Anomalous neutron yields confirmed for Ba-Mo and newly observed for Ce-Zr from spontaneous fission of Cf 252

We reinvestigated the neutron multiplicity yields of Ba-Mo, Ce-Zr, Te-Pd, and Nd-Sr from the spontaneous fission of 252 Cf by (i) using both γ -γ -γ -γ and γ -γ -γ coincidence data, (ii) using up to date level scheme structures, and (iii) crosschecking analogous energy transitions in multiple isotopes, we have achieved higher precision than previous analyses. Particular attention was given to the Ba-Mo pairs where our results clearly confirm that the Ba-Mo yield data have a second hot fission mode where 8–10, and now 11 neutron evaporation channels are observed. These are the first observations of the 11 neutron channel. These 8–11 neutron channels are observed for the first time in the Ce-Zr pairs, but are not observed in other fission pairs. The measured intensities of the second mode in Ba-Mo and Ce-Zr pairs are ~1.5(4)% and ~1.0(3)%, respectively. These high neutron number evaporation modes can be an indication of hyperdeformation and/or octupole deformation in 143-145 Ba and in 146,148 Ce at scission to give rise to such high neutron multiplicities.

252-Cf↗

An Artificial Neural Network System for Photon-Based Active Interrogation Applications

Active interrogation (AI) is a promising technique to detect shielded special nuclear materials (SNMs). At the University of Michigan, we are developing a photon-based AI system that uses bremsstrahlung radiation from an electron linear accelerator (linac) as an ionizing source and stilbene organic scintillating detectors for neutron detection. Stilbene scintillators are sensitive to fast neutrons and photons and have excellent pulse shape discrimination (PSD) capabilities. The traditional charge integration (CI) method commonly used for PSD analysis eliminates piled-up pulses and relies on a particle discrimination line to separate neutrons and photons. The presence of the intense photon flux during AI creates a significant number of piled-up events in the stilbene scintillator, thereby posing a great challenge to the traditional CI method. Identifying true single neutron pulses becomes challenging due to the presence of a pile-up cloud and overlapping neutron, photon and pile-up clouds in the PSD analysis. To mitigate the effect of pulse pile up and identify true single neutron pulses from stilbene scintillators, an artificial neural network (ANN) system is developed. The developed ANN system identifies single neutron pulses and neutron-photon combinations from piled-up events. The results obtained from a 252Cf measurement in the presence of the intense photon flux show that the developed ANN system outperforms the traditional CI method. Since many piled-up events lie above the particle discrimination line, they get misclassified as neutrons by the traditional CI method resulting in 25% overestimation of the net neutron count rate during the linac pulse. The overall net neutron count rate (single and restored neutrons) during the linac pulse, estimated by the ANN system is 60% of the ground truth. Energy spectroscopy of the ANN attributed single neutron pulses further provides evidence on the detection of prompt fission neutrons from the 252Cf fission source.

42 ENGINEERING↗

Evaluation of Niowave's Proposed Solvent Washing Approach

Niowave, Inc., is a domestic supplier of medical and industrial isotopes from uranium (U) and radium (Ra). The company has recently entered into a cooperative agreement with the U.S. Department of Energy’s National Nuclear Security Administration (NNSA) and plans to deploy a superconducting electron accelerator (LINAC) to fission U for molybdenum-99 ( 99 Mo) production without the need for a nuclear reactor or highly enriched uranium (HEU). NNSA provided funding to the Savannah River National Laboratory (SRNL) to support Niowave in this effort. SRNL evaluated the application of the solvent washing process for Niowave.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

To Mars in 30 days by gas-core nuclear rocket.

An important component for a concept involving a 60-day Mars mission is the gas-core nuclear-rocket engine. A gas-core reactor, however, has also other potential applications including MHD power generators, breeder reactors, and nuclear-powered lasers. The gas-core engine uses a fissioning uranium plasma to heat hydrogen and then expands it through a nozzle to convert the thermal energy into thrust. To obtain a higher specific impulse than the 825 sec of the solid-core nuclear-rocket engine, a gas core has to produce hotter hydrogen.

Ragsdale, R. G.↗

Experimental Studies of NaK in a Simulated Space Environment

Space fission power systems are being developed at the National Aeronautics and Space Administration (NASA) and Department of Energy (DOE) with a short term goal of building a full scale, non-nuclear, Technology Demonstration Unit (TDU) test at NASA's Glenn Research Center. Due to the geometric constraints, mass restrictions, and fairly high temperatures associated with space reactors, liquid metals are typically used as the primary coolant. A eutectic mixture of sodium (22 percent) and potassium (78 percent), or NaK, has been chosen as the coolant for the TDU with a total system capacity of approximately 55 L. NaK, like all alkali metals, is very reactive, and warrants certain safety considerations. To adequately examine the risk associated with the personnel, facility, and test hardware during a potential NaK leak in the large scale TDU test, a small scale experiment was performed in which NaK was released in a thermal vacuum chamber under controlled conditions. The study focused on detecting NaK leaks in the vacuum environment as well as the molecular flow of the NaK vapor. This paper reflects the work completed during the NaK experiment and provides results and discussion relative to the findings.

Gibons, Marc↗

Performing k eff Validation of As-Loaded Criticality Safety Calculations Using UNF-ST&DARDS: Sensitivity Calculations

The general method for performing validation of as loaded criticality safety calculations using UNF ST&DARDS is presented in a paper by Clarity, which includes a description of the UNF-ST&DARDS system. Proof-of-principle analyses were performed in the summer of 2019 for MPC-32 dual purpose canisters (DPCs) containing pressurized water reactor (PWR) fuel assemblies. Summaries of these results are presented in this and a companion paper for this conference. The current paper describes the TSUNAMI-3D calculations performed to generate sensitivity data, and the companion paper discusses the selection of critical experiments applicable for validation of the 11 MPC-32 DPCs considered. The generation of sensitivity data for as-loaded spent nuclear fuel (SNF) DPCs is a challenge given the detailed model of the fuel compositions generated by UNF ST&DARDS. Each fuel assembly is modeled with its own irradiation history in 18 axial nodes, unless the fuel assembly is damaged and thus considered as fresh by design basis. This results in a set of 576 fuel compositions, each of which must be processed separately in a multigroup (MG) calculation. Therefore, a continuous-energy (CE) TSUNAMI-3D method was chosen to alleviate this challenge. Two CE TSUNAMI-3D methods are available in SCALE 6.2.3: the iterated fission probability (IFP) and contribution-linked eigenvalue sensitivity/uncertainty estimation via track-length importance characterization (CLUTCH). Since the IFP method is not feasible because of memory requirements associated with its implementation in SCALE, the CLUTCH method was selected for these calculations. CLUTCH has been implemented in SCALE in parallel, allowing long calculations to be performed in reasonable timeframes. The two primary user inputs necessary for CLUTCH calculations are the F*(r) mesh and the number of latent generations used in determining the F*(r) function. This F*(r) function is used as the importance function for fission chains originating in a given volume element (voxel), and it is calculated using the IFP method in the skipped generations. A large number of skipped generations is thus required to ensure accurate calculation of this importance function. In these calculations, 500 generations were used to calculate the F*(r) function. For more information regarding the calculation of F*(r), see Jones [4]. The remainder of this paper is focused on the selection of the F*(r) mesh and the number of latent generations.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Simulated Energy Response in a Multiplicity Detector

Neutron multiplicity analysis is used for many applications, including nonproliferation and criticality safety. Multiplicity detectors have advantages over total neutron counting as they provide the ability to assess both multiplication and mass in fissionable material. In addition, multiplicity detectors can generate real-time information, e.g., dose estimation. The ability to evaluate the detector efficiency in each application is of primary importance in producing meaningful analyses. Multiplicity detectors usually house 3 He tubes within a polyethylene moderator. If the tubes are located behind different thickness of polyethylene, they will have different energy responses. This paper assesses 3 He tube efficiency as a function of neutron energy for a specific multiplicity detector.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗