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Spectroscopic data for all nuclei with mass number A=47 have been evaluated and the corresponding level schemes from radioactive decay and reaction studies are presented. Highlights from this evaluation include first observation of gamma-ray transitions in 47 Ar, a new high precision measurement of 47 K β decay, and first observation of excited levels and gamma-ray transitions in 47 Mn.
In advanced reactor (AR) designs, a common feature is continuous chemical processing and circulation of the nuclear material. This work bridges a significant measurement gap in safeguarding reactors with circulating fuel or continuous refueling by leveraging and building on the isotope ratio method first developed by our team under an FY21 Advanced Reactors International Safeguards Engagement (ARISE) project (Uribe et al. 2021). In circulating fuel designs, the radioisotope inventory changes from traditional effects (e.g., radioactive decay, fission) but also includes material transport due to pressure and temperature gradients. Such designs may also require regular or continuous additions or removals during operation, which significantly increases the rate of inventory change compared to traditional pressurized water reactor (PWR)s. Thus, directly tracking the nuclear inventory is ineffective since the isotopes are continuously added and removed. The isotope ratio method instead focuses on detecting changes to the input and output flows of radioisotopes. Previous work showed that for well-chosen pairs of isotopes, the isotopic ratio provides a sensitive and lasting indicator of deviation from normal conditions (e.g., startup, shutdown, diversion). The isotope ratio method is a process monitoring method with potential for application in for forward-looking approaches to International Atomic Energy Agency (IAEA) safeguards. The original process monitoring method was developed for a specific case—the decay tank of a thorium-fueled molten salt breeder reactor. In this expanded work, we explored other types of reactors and processes with nonstationary (e.g., flowing) nuclear material, which are difficult to safeguard with traditional methods because of the transient nature of the systems. The goal of the present work is to generalize the isotope ratio method for use in processes with continuously flowing nuclear material. All continuous processes have an average time for isotopes to be replaced in the system. The isotope ratio method works by choosing radioisotopes with half-lives both above and below the processing time. The present work seeks to explore which isotopes are suitable for the method by simulating the nuclear inventory, radioisotope emissions, and detector responses for several classes of advanced reactors. While the method can in principle be applied to other processes (e.g., enrichment or reprocessing facilities), the present work limits scope to ARs with continuously flowing fuel. Section 2 details the mathematics supporting the isotope ratio method, and Section 3 introduces the representative ARs selected for this work. Section 4 discusses how each reactor was analyzed, and Section 5 showcases the results for each representative reactor. Finally, Section 6 provides concluding remarks and suggests pathways for further analysis.
Betavoltaics (BV) are long-life power sources that typically convert beta particle radiation into electricity. Largely, the radioactive decays within the source go unharvested by the device. This work seeks to augment the power generation of BV devices by integration of scintillating particles within the radiative getter to convert beta emission which would otherwise not leave the getter into usable light for power generation. Silica-covered barium fluoride scintillating particles were integrated into a tritiated water getter. Power generation was increased from 100s of nW to µW levels with the addition of 0.2 wt. % particles into the getter. Nanowatt-scale sensor platforms were demonstrated with the µW BV devices and the maximum possible lifetime of such platforms was estimated. As this technique enables higher power density BV devices from conventional Si semiconductors (compared to wider bandgap BVs), the further implementation may lower the barrier-to-deployment of these long-life power/sensor platforms.
This study measured radiolytic gas generation and pressure buildup in a sealed stainless-steel system containing alkaline Mo-99 solution with added sodium nitrate as a hydrogen suppressant. In each of two experiments, approximately 200 Ci of Mo-99 solution was transferred into a closed experimental vessel inside a hot cell, isolated, and monitored for pressure rise caused by gas generation during radioactive decay. After pressure buildup, headspace gas samples were collected and analyzed by mass spectrometry to determine hydrogen and oxygen concentrations. The purpose was to quantify the magnitude of pressure buildup in a closed system and to characterize the gas composition produced by radiolysis of the Mo-99 target solution under representative handling and storage conditions. The two experiments used similar total Mo-99 activity but differed in solution volume, headspace volume, and leak integrity. In the first experiment, 197.5 Ci of Mo-99 in 16.92 mL of solution was loaded into a vessel with a 31.1-mL headspace; a small leak was later identified, and the measured peak pressure of 46 psig was extrapolated to about 70 psig in the absence of leakage. The headspace gas from this experiment contained about 21.4% H2 and 63.4% O2, but the composition was influenced by preferential hydrogen loss through the leak. In the second experiment, 193 Ci of Mo-99 in 5.41 mL of solution with 0.46 g NaNO3 was loaded into a vessel with a larger 42.61 mL headspace, and no detectable leak was observed. This experiment reached a peak pressure of 38 psig, and the measured gas composition was approximately 28.2% H2 and 51.5% O2. Because the second experiment was leak-free, it is considered the more reliable indicator of the true pressure buildup and intrinsic radiolytic gas composition of the Mo-99 solution.
Abstract Type IIP supernovae (SNe IIP) are thought to originate from the explosion of massive stars >10M ⊙ . Their luminosity is primarily powered by the explosion energy and the radioactive decay energy of 56 Co, with the photosphere location regulated by hydrogen recombination. However, the physical connections between SNe IIP and their progenitor stars remain unclear. This paper presents a comprehensive study of SNe IIP and their progenitor stars by using the one-dimensional stellar evolution code,MESA. Our model grids consider the effects of stellar metallicity, mass, and rotation in the evolution of massive stars, as well as the explosion energy and 56 Ni production in modeling supernovae. To elucidate the observed SNe IIP and their origins, we compare their light curves (LCs) with our models. Furthermore, we investigate the impact of stellar parameters on LCs by considering stellar mass, metallicity, rotation, explosion energy, and 56 Ni production. We find that more massive stars exhibit longer plateaus due to increased photon diffusion time caused by massive ejecta. Higher metallicity leads to increased opacity and mass loss of progenitor stars. Rapid rotation affects internal stellar structures, enhancing convective mixing and mass loss, potentially affecting the plateau’s brightness and duration. Higher explosion energy results in brighter but shorter plateaus due to faster-moving ejecta. 56 Ni mass affects late-time luminosity and plateau duration, with larger masses leading to slower declines.
The precise atomic structure and therefore the wavelength-dependent opacities of lanthanides are highly uncertain. This uncertainty introduces systematic errors in modeling transients like kilonovae and estimating key properties such as mass, characteristic velocity, and heavy metal content. Here, we quantify how atomic data from across the literature as well as choices of thermalization efficiency of r-process radioactive decay heating impact the light curve and spectra of kilonovae. Specifically, we analyze the spectra of a grid of models produced by the radiative transfer code Sedona that span the expected range of kilonova properties to identify regions with the highest systematic uncertainty. Our findings indicate that differences in atomic data have a substantial impact on estimates of lanthanide mass fraction, spanning approximately 1 order of magnitude for lanthanide-rich ejecta, and demonstrate the difficulty in precisely measuring the lanthanide fraction in lanthanide-poor ejecta. Mass estimates vary typically by 25%–40% for differing atomic data. Similarly, the choice of thermalization efficiency can affect mass estimates by 20%–50%. Observational properties such as color and decay rate are highly model dependent. Velocity estimation, when fitting solely based on the light curve, can have a typical error of ∼100%. Atomic data of light r-process elements can strongly affect blue emission. Even for well-observed events like GW170817, the total lanthanide production estimated using different atomic data sets can vary by a factor of ∼6.
We present far- and near-ultraviolet (UV) spectra of the type II supernovae (SNe) SN 2023ixf from days 199 to 722 and SN 2024ggi at days 41 and 232. Both SNe show broad, blueshifted, and asymmetric UV emission lines with an initial maximum velocity of ∼9000 km s −1 and narrow unresolved emission in C ivλλ1548.9, 1550.8. We compare the optical and UV emission-line profiles, showing that they evolve from two distinct velocity profiles to a single profile tracing the UV emission. We interpret this as shock power from interaction with circumstellar material coming to dominate over the radioactive-decay power from the inner ejecta. Comparing our observations to radiative transfer models with injected shock power, we find SN 2024ggi is best matched by P shock,abs = 1 × 10 41 erg s −1 at day 40; SN 2023ixf at day 300 and SN 2024ggi at day 200 are best matched by P shock,abs = 1 × 10 40 erg s −1 ; and SN 2023ixf at day 600 is best matched by Pshock,abs = 5 × 10 39 erg s −1 . From these models, we find that the mass-loss rate of both SNe increased just before the explosion. For SN 2023ixf, our mass-loss rates go from 4 × 10 −5 M ⊙ yr −1 at 600 yr before explosion to 2 × 10 −2 M ⊙ yr − 1 at 15 yr prior to explosion. For SN 2024ggi, we find a mass-loss rate of 9 × 10 −5 M ⊙ yr −1 at 150 yr before explosion and 1 × 10 −3 M ⊙ yr −1 at 30 yr before explosion.
The radioactive decay of unstable nuclei created in the rapid neutron capture process releases a large amount of γ-rays. When the ejecta are optically thick, these γ-rays may contribute to an associated kilonova. Once transparent, prominent spectral features will be directly observable in current and future γ-ray detectors. In this work, we study and compare the γ-ray spectra of different representative r-process trajectories across a broad range of timescales, from hours to 50,000 yr, identifying the nuclei that significantly contribute. We discuss these findings in the context of observability, noting that there are several practical challenges to connecting observed signatures to specific nuclei. However, if these challenges can be overcome, direct observation of γ-rays from r-process sites can provide insight into the fundamental physics underpinning the r-process.
The fuel performance modeling code BISON was used to predict the release of fission products iodine-131 (131I), xenon-133 (133Xe), and krypton-85 (85Kr) from four re-irradiated AGR-3/4 fuel compacts containing tristructural isotropic (TRISO) coated particles during high-temperature isothermal heating tests. The AGR-3/4 fuel compacts were irradiated in the Advanced Test Reactor (ATR) as part of the third and fourth series of planned experiments to support the Advanced Gas Reactor (AGR) Program. They were subsequently stored and re-irradiated in the Neutron Radiography (NRAD) reactor for approximately five days and then stored for another five to eight days before being subjected to isothermal heating tests in the Fuel Accident Condition Simulation (FACS furnace) for 200 to 300 hours at temperatures between 1000°C and 1600°C to evaluate fission product release at elevated temperatures. New nuclide-specific fission product source term models for the three nuclides of interest were developed using the reactor multiphysics code Griffin and implemented into BISON to support this work. The new source term models were incorporated into coupled compact- and particle-scale BISON simulations, which predict spatially- and temporally-resolved radionuclide generation, radioactive decay, transport, and release throughout the entire irradiation history, including the initial ATR irradiation, NRAD re-irradiations, FACS heating tests, and intermediate periods spent in storage. The experimentally measured fission product release from the heating tests were compared to modeling release predictions calculated by BISON to evaluate how well the code compares to experimental results. Overall, the experimental measured and BISON predicted comparative release results varied but generally agreed to within 5 particle equivalents. Comparative release results identified general observations to take into consideration to help refine future models and reduce uncertainties associated with both the measurement results and predictive results. This includes developing new uranium oxycarbide (UCO) specific kernel diffusivities for the three isotopes examined to more accurately reflect the material properties of the fuel form. Deriving new diffusivities will aid in producing a more informed BISON model
Plutonium plays a critical role in nuclear fuel cycle technologies, but our understanding of its fundamental radiation-induced redox chemistry is limited. Changes in oxidation states affect the speciation and transport of plutonium ions in solution. For example, solvent extraction techniques used to separate and recover plutonium from used nuclear fuel rely on the selective formation, maintenance, and complexation of specific plutonium oxidation states. However, radiolytically generated radicals, ions, and molecules can drive the oxidation state distribution of plutonium ions far from equilibrium, ultimately changing the physical and chemical properties of the bulk system. These radiation-induced processes are inevitable due to the ionizing radiation fields generated by the radioactive decay of plutonium and its daughter nuclides. Therefore, mechanistically understanding how plutonium's various oxidation states respond to ionizing radiation is essential for predicting its behavior in solution. Here, we present significant advances in our understanding of radiation-induced plutonium redox chemistry by using time-resolved (electron pulse) and dose accumulation (alpha and gamma) irradiation techniques, along with quantitative multiscale modeling methods.
The concept of measuring neutron flux (or fluence rate) with activation foils has existed since the late 1940s and is a well-used methodology. Activation foils are selected for their unique isotopic cross sections that create reaction products with desirable properties: relatively simple radioactive decay scheme, measurable quantities of gamma-rays or betas, and half-lives appropriate for the irradiation and decay durations of the experiment. The activation materials, deemed flux wires, fluence wires, dosimeters, or flux foils, are fabricated to have a mass appropriate for the irradiation as well so the measurement using a radiation detector following the irradiation is sufficient but not overwhelming in terms of total activity. Activation measurement results are expressed in terms of reaction rate, which can then be used to “adjust” the neutron spectrum. The Advanced Graphite Creep (AGC)-4 experiment contained 26 flux wire packages, each containing an iron and a niobium wire inside a vanadium capsule. For all stackup positions, the value of fast to thermal neutrons is higher than expected, but the total neutron fluence is near the predicted value of ~2 x 1022 n/cm2. As compared to the predicted neutron spectrum, there are four takeaways in the results as compared to the predicted ATR irradiation: 1) Additional fast (fission) neutrons present, 2) Spectrum hardening due to temperature, 3) Spectrum hardening due to container attenuation, 4) Total neutron fluence is close to predicted values. Since the neutron energy spectrum is a key parameter when attributing neutron damage in materials, the adjusted energy-dependent spectrum and the total neutron fluence results from the dosimeters can be incorporated for future calculations.
Context . The 1.8 MeV γ -rays corresponding to the decay of the radioactive isotope 26 Al (with a half-life of 0.72 Myr ) have been observed by the SPI detector on the INTEGRAL spacecraft and extensively used as a tracer of star formation and current nucleosynthetic activity in the Milky Way Galaxy. Further information is encoded in the observation related to the higher 26 Al content found in regions of the Galaxy with the highest line-of-sight (LoS) velocity relative to an observer located in the Solar System. However, this feature remains unexplained. Aims . We ran a cosmological “zoom-in” chemodynamical simulation of a Milky Way-type galaxy, including the production and decays of radioactive nuclei in a fully self-consistent way. We then analyzed the results to follow the evolution of 26 Al throughout the lifetime of the simulated galaxy to provide a new method for interpreting the 26 Al observations. Methods . We included the massive star sources of 26 Al in the Galaxy and its radioactive decay into a state-of-the-art galactic chemical evolution model, coupled with cosmological growth and hydrodynamics. This approach allowed us to follow the spatial and temporal evolution of the 26 Al content in the simulated galaxy. Results . Our results are in agreement with the observations with respect to the fact that gas particles in the simulation with relatively higher 26 Al content also have the highest LoS velocities. On the other hand, gas particles with relatively lower 26 Al content (i.e., not bright enough to be observed) generally display the lowest LoS velocities. However, this result is not conclusive because the overall rotational velocity of our simulated galaxy is higher than that observed for cold CO gas in the Milky Way Galaxy. Furthermore, we found no significant correlation between gas temperature, rotational velocity, and 26 Al content at any given radius. We also found the presence of transient 26 Al-rich spots at low LoS velocities and we show that one such spot had been captured by the INTEGRAL/SPI data. Based on our model, we present a prediction for the detection of 1.8 MeV γ -rays by the future COSI mission. We find that according to our model, the new instrument will be able to observe similar 26 Al-emission patterns to those seen by INTEGRAL/SPI.
There are programs for high-Z shell experiments at the National Ignition Facility (NIF). For shells made of actinide material, a quantitative fission diagnostic is needed in order to determine how much fission took place and whether the fission was sufficient to produce a non-negligible heat source in the burning capsule. Here, we present a viable coupled experimental and theoretical technique for making quantitative fission measurements possible. The proposed scheme involves using a well-characterized set of depleted uranium foils outside an NIF capsule to verify the conversion of xenon and krypton fission fragments collected at the Radiochemical Analysis of Gaseous Samples (RAGS) facility into total fission yield. We present the calculations needed for this conversion, including the decays in and out of fission fragment chains during the RAGS pump-down of the NIF chamber.
There is a growing realization that neutrinos can be used as a diagnostic tool to better understand the inner workings of a nuclear weapon. Robust estimates demonstrate that an Inverse Beta Decay (IBD) neutrino scintillation detector built at the Nevada Test Site with a 1000-ton active target mass at a standoff distance of 500 m would detect thousands of antineutrino events per nuclear test. This would provide less than 4% statistical error on the measured antineutrino rate and 5% error on antineutrino energy. Extrapolating this to an error on the test device explosive yield requires knowledge from evaluated nuclear databases, non-equilibrium fission rates, and assumptions on internal neutron fluxes. Initial calculations demonstrate that the total number of neutrinos emitted per fission in the first 10 3 s after a short pulse of 239 Pu fission is about a factor of two less than that from Pu fissioning under steady state conditions. Furthermore, there are significant energy spectral differences as a function of time after the pulse that must be considered. These and other model dependencies will be discussed in the paper. In the absence of nuclear weapons testing, many of the technical and theoretical challenges of a full nuclear test could be mitigated with a low cost smaller scale 20 ton fiducial mass IBD demonstration detector placed near a pulsed reactor. Potential reactors include the Texas A&M University TRIGA 1 GW–10 ms pulsed facility or the Sandia Annular Core Research Reactor. The short duty cycle and repeatability of pulses would provide critical real environment testing and measurements, which would be valuable for planning a possible real test shot in the future. Furthermore, the antineutrino rate as a function of time data would provide unique constraints on fission databases and model assumptions. Finally, there are impactful science drivers such as sensitive searches for ∼1 eV 2 sterile neutrinos and ∼MeV scale axions.
The fragmentation of molecular cations following inner-shell decay processes in molecules containing heavy elements underpins the X-ray damage effects observed in X-ray scattering measurements of biological and chemical materials, as well as in medical applications involving Auger electron-emitting radionuclides. Traditionally, these processes are modeled using simulations that describe the electronic structure at an atomic level, thereby omitting molecular bonding effects. This work addresses the gap by introducing a novel approach that couples Auger–Meitner decay to nuclear dynamics across multiple decay steps, by developing a decay spawning dynamics algorithm and applying it to potential energy surfaces characterized with ab initio molecular dynamics simulations. We showcase the approach on a model decay cascade following K-shell ionization of IBr and subsequent Kβ fluorescence decay. We examine two competing channels that undergo two decay steps, resulting in ion pairs with a total 3+ charge state. This approach provides a continuous description of the electron transfer dynamics occurring during the multistep decay cascade and molecular fragmentation, revealing the combined inner-shell decay and charge transfer time scale to be approximately 75 fs. In conclusion, our computed kinetic energies of ion fragments show good agreement with experimental data.
Radioactive sources can provide power in remote and environmentally harsh locations such as the arctic or space. The generators powered by such sources are rugged and can withstand extreme temperatures, lack of sunlight, and require no human intervention for multiple years. Radioisotopes are used in thermoelectric generators to provide power at remote sites and deep in space. Isotopes like Pu-238, Cm-244, and Am-241 are used in these generators by NASA for power in space probes and spacecrafts. These power sources deliver a steady supply of energy over extended periods of time. Alpha particles created during decay do not travel far in a material. Their kinetic energy is transferred to heat that we can then convert into energy. Unlike beta and gamma decay, the slower-moving alpha particles stop in the material, making their energy available for use. Energy from these natural decay processes provides a reliable source of power. Spontaneous fission is rare and unreliable, and unlike induced fission processes, alpha decay occurs naturally and does not require external management or ignition. The ideal properties of an isotope for use as a power source depend upon the intended use. For use in an Arctic research base over a period of several years, but less than a decade, an isotope that provides high power output over a shorter lifespan may be the most suitable option. Whereas, for deep space missions where a consistent power source for decades or perhaps more than 100 years is needed that would require a very different isotope. One with a much longer half-life that would provide consistent power throughout that time and survive in that state in for these extended periods of time. These examples represent two extreme sides in terms of time frames. By analyzing the power produced by different radioactive decay processes over time, we can evaluate the suitability of various isotope decay chains for specific uses. Some unstable isotopes undergo a series of radioactive decays, transforming into different isotopes at each step and resulting in a stable isotope. The lists of isotopes in these decay processes are known as decay chains. Some of these chains, illustrated in the figures below, are currently being investigated for use in radioisotope thermoelectric generators (RTGs) designed for a range of operational durations.
The ability to differentiate between atmospheric radionuclide signatures from underground nuclear explosions (UNEs) and signals from other sources, such as medical isotope-production facilities and nuclear reactors, can be critical to the detection and monitoring of unannounced, low-yield nuclear events. Signatures having anomalously high amplitudes, compared to background levels, remain the best indicator in screening for a UNE. However, isotopic composition can further validate a suspected UNE signature, but separation from any atmospheric background composition is first necessary. To date, evaluating the challenges of performing this separation has typically involved comparing an observed background with a highly idealized deterministic model of radioxenon signature production by a UNE that does not consider the influence of post-detonation chemical/physical processes in the detonation cavity or the subsequent gas transport mechanisms that can also affect the isotopic composition of the detected gas signature. In addition, purely deterministic models, as previously employed, overlook the uncertainty inherent in estimating critical parameters characterizing the UNE and its detonation environment. In this paper, we create detailed, multi-parameter models of radionuclide evolution using the widely accepted England and Rider post-detonation radionuclide decay-chain network coupled to detailed models simulating physical production and transport processes affecting the gas signature. Because these models are governed by uncertain parameters including barometric fluctuations, realistic ranges of variation for each of the parameters influencing isotopic composition are then defined. A Latin-Hypercube sampling approach is used to obtain a random distribution of isotopic production and gas transport results associated with a given value of each parameter. We apply these results to background histories of two stations, one providing 4-isotope background measurements and the other providing two-isotope measurements associated with the 2013 DPRK announced UNE.
A rate theory for void and bubble swelling is derived that allows both vacancies and self-interstitial atoms to be generated by thermal activation at all sinks. In addition, they can also be produced by displacement damage from external and internal radiation. This generalized rate theory (GRT) is applied to swelling of gallium-stabilized δ-plutonium in which α-decay causes the displacement damage. Since the helium atoms produced also become trapped in vacancies, a distinction is made between empty and occupied vacancies. The growth of helium bubbles observed by transmission electron microscopy in weapons-grade and in material enriched with Pu238 is analyzed, using different values for the formation energy of self-interstitial atoms (SIA) and two different sets of relaxation volumes for the vacancy and for the SIA. One set allows preferential capture of SIA at dislocations, while the other set gives equal preference to both vacancy and SIA. It is found that the helium bubble diameters observed are in better agreement with GRT predictions if no preferential capture occurs at dislocations. Therefore, helium bubbles in δ-plutonium will not evolve into voids. Furthermore, the helium density within the bubbles remains sufficiently high to cause thermal emission of SIA. Based on a helium density between two to three helium atoms per vacant site, the sum of formation and migration energies must be around 2.0 eV for SIA in δ-plutonium.