Noble Gas Capture [Slides]
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Oak Ridge National Laboratory completed the resolved resonance region (RRR) evaluation of the two most abundant cerium isotopes, 140 Ce (88.45%) and 142 Ce (11.11%), as requested by the US Nuclear Criticality Safety Program. These evaluations are based on recent high-resolution transmission and capture measurements performed on nat Ce and highly enriched 142 Ce samples at the JRC-Geel Linear Accelerator facility, as well as measured thermal constants available from the EXFOR database. Starting from the resonance parameters of the ENDF/B-VIII.0 library followed by a preliminary R-matrix analysis, an updated set of resonance parameters and corresponding covariance information were derived by fitting these measured data using the Reich–Moore approximation of the R -matrix theory, as implemented in the SAMMY code system. The 140 Ce RRR upper energy limit was kept at 200 keV, whereas the 142 Ce resonance region was extended from 13 to 26 keV. Updated statistical properties were obtained for the new evaluations and compared to those derived from the ENDF/B-VIII.0 nuclear data library. The new evaluation work improved some of the discrepancies found in previous work, such as the capture resonance integral and stellar Maxwellian-averaged cross sections. These integral quantities were mainly derived from the fit of the latest measured data, especially the neutron capture yield data for 142 Ce isotope.
The release of radioiodine, one of several radionuclides of concern when recycling used nuclear fuel (UNF), is an important consideration in the fuel cycle. In this study, two sorbent materials, Cu 0 -polyacrylonitrile (PAN) and Bi 0 -PAN, were tested as solid sorbent candidates for iodine capture. Experiments using a thin bed of sorbent material were exposed to vaporized iodine for over 300 hours (~2 weeks) under varied conditions in a dynamic flow environment. The overall performance was monitored in real-time using thermogravimetric analysis, and the materials were subsequently characterized for surface and bulk analysis using scanning electron microscopy – energy-dispersive spectroscopy (SEM-EDS) and powder x-ray diffraction (pXRD), respectively. Iodine (in the form of I 2 ) is expected to be released primarily in the dissolver off-gas (DOG) stream; therefore, this study demonstrates the effects of elemental iodine (I 2 ), water vapor (H 2 O), and nitrogen dioxide (NO 2 ). When exposed to ‘ideal’ conditions (in which I 2 is carried by dry air), Cu 0 -PAN and Bi 0 -PAN behave differently, with TGA analysis indicating that Cu 0 sorption performance is higher than that of Bi 0 , as evidenced by a larger mass change. Under ‘harsh’ conditions—such as a gaseous feed containing I 2 , H 2 O, and NO 2 vapors carried by air,—iodine capture performance for both Cu 0 - and Bi 0 -PAN are affected. SEM-EDS and pXRD analysis of these materials is discussed herein.
In this article, we provide an overview of state-of-the-art techniques that are being developed for efficient calculation of second and higher nuclear derivatives of quantum mechanical (QM) energy. Calculations of nuclear Hessians and anharmonic terms incur high costs and memory and scale poorly with system size. Three emerging classes of methods—machine learning (ML), automatic differentiation (AD), and matrix completion (MC)—have demonstrated promise in overcoming these challenges. We illustrate studies that employ unsupervised ML methods to reduce the need for multiple Hessian calculations in dynamics simulations and those that utilize supervised ML to construct approximate potential energy surfaces and estimate Hessians and anharmonic terms at reduced cost. By extension, if electronic structure operations could be written in a manner similar to functions underlying ML methods, rapid differentiation or AD routines can be employed to inexpensively calculate higher arbitrary-order derivatives. While ML approaches are typically black-box, we describe methods such as compressed sensing (CS) and MC, which explicitly leverage problem-specific mathematical properties of higher derivatives such as sparsity and low-rank, to complete higher derivative information using only a small, incomplete sample. The three classes of methods facilitate reliable predictions of observables ranging from infrared spectra to thermal conductivity and constitute a promising way forward in accurately capturing otherwise intractable higher-order responses of QM energy to nuclear perturbations.
Heavy-ion storage rings have relatively large momentum acceptance which allows for multiple ion species to circulate at the same time. This needs to be considered in radioactive decay measurements of highly charged ions, where atomic charge exchange reactions can significantly alter the intensities of parent and daughter ions. In this study, we investigate this effect using the decay curves of ion numbers in the recent 205 Tl 81+ bound-state beta decay experiment conducted using the Experimental Storage Ring at GSI Darmstadt. To understand the intricate dynamics of ion numbers, we present a set of differential equations that account for various atomic and nuclear reaction processes—bound state beta decay, atomic electron recombination and capture, and electron ionization. By incorporating appropriate boundary conditions, we develop a set of differential equations that accurately simulate the decay curves of various simultaneously stored ions in the storage ring: 205 Tl 81+ , 205 Pb 81+ , 205 Pb 82+ , 200 Hg 79+ , and 200 Hg 80+ . Through a quantitative comparison between simulations and experimental data, we provide insights into the detailed reaction mechanisms governing stored heavy ions within the storage ring. Our approach effectively models charge-changing processes, reduces the complexity of the experimental setup, and provides a simpler method for measuring the decay half-lives of highly charged ions in storage rings.
Neutron-induced reaction cross sections of short-lived nuclei are imperative to understand the origin of heavy elements in stellar nucleosynthesis and for societal applications, but their measurement is extremely complicated due to the radioactivity of the targets involved. One way of overcoming this issue is to combine surrogate reactions with the unique possibilities offered by heavy-ion storage rings. In this work, we describe the first surrogate-reaction experiment in inverse kinematics, which we successfully conducted at the Experimental Storage Ring (ESR) of the GSI/FAIR facility, using the 208 Pb(p,p') reaction as a surrogate for neutron capture on 207 Pb. Thanks to the outstanding detection efficiencies possible at the ESR, we were able to measure for the first time the neutron-emission probability as a function of the excitation energy of 208 Pb. We have used this probability to select different descriptions of the γ -ray strength function and nuclear level density, and provide reliable results for the neutron-induced radiative capture cross section of 207 Pb at energies for which no experimental data exist.
This module will provide an overview of best practices for nuclear security planning requirements to include building a nuclear security plan and a concept of operations. It will introduce best practices for nuclear security planning to include the following: (1) Develop a Nuclear Security Plan, (2) Review 10 key elements of a Concept of Operations, (3) Estimate resources for an MPE, and (4) Capture lessons learned and best practices.
A unique attribute of the nuclear industry is the extent by which designers, developers, operators, and regulators pay attention to demonstrating the safety case. The safety case for nuclear systems is a written, traceable expression of safety, demonstrating the system’s protective measures against uncontrolled radiological releases. The nuclear installation resiliency or safety takes overriding priority over function and performance. The preparation of the safety case heavily relies on extensive experimental campaigns that challenge the target design under a spectrum of postulated accident scenarios. For safety reasons, these experiments are typically conducted in sub-scale test apparatuses intended to reproduce the postulated accident scenarios and event sequences realistically but subject to proven similarity criteria, often referred to as scaling analyses. Since the dawn of the nuclear industry, significant resources have been committed to the construction and operation of such test facilities and a massive amount of data has been generated. Such test data have been and are still used to validate the fundamental assumptions of nuclear power plant phenomena. As we move into the digital world, capturing this multi-decades worth of information in a transparent, easily accessible, and usable manner for the public and industry stakeholders is of paramount importance. Over the last few years FPoliSolutions has been actively developing an enterprise digital data ontology platform (FPoliDON) intended to do just that. The concept was introduced in a paper at the previous NURETH edition and has been significantly enhanced since. With the vision of helping designers use the data to assess their safety case evaluation models, the platform was designed not only to ontologically organize the experimental data, but also to guide the user in the complex analytics associated with the interpretation and use of such test results. A new feature which has been recently added is the ability for the user to access a library of sophisticated mathematical procedures for performing scaling analyses. For this purpose, the Dynamical System Scaling (DSS) procedure invented by Dr. Jose’ Reyes was formulated as one of the services in the digital platform. These methods have been demonstrated to provide an excelled mathematical apparatus to identify similarity criteria or quantify distortions between measured data and the target prototypical conditions. Moreover, DSS can provide a level of synthesis across SETs and IETs which has the promise to yield efficiency in the evaluation code assessment activities. This is often a daunting and expensive task to set up evaluation models that support the safety case of current and future nuclear power plants.
Potassium-40 is a widespread, naturally occurring isotope whose radioactivity impacts subatomic rare-event searches, nuclear structure theory, and estimated geological ages. A predicted electron-capture decay directly to the ground state of argon-40 has never been observed. Here, the KDK (potassium decay) collaboration reports strong evidence of this rare decay mode. A blinded analysis reveals a nonzero ratio of intensities of ground-state electron-captures (I EC 0 ) over excited-state ones (I EC $\star$ ) of I EC 0 /I EC $\star$ = 0.0095 $^{stat}_{±}$ 0.0022 $^{sys}_{±}$ 0.0010 (68% C.L.), with the null hypothesis rejected at 4σ. In terms of branching ratio, this signal yields I EC 0 = 0.098 % $^{stat}_{±}$ 0.023 % $^{sys}_{±}$ 0.010 % , roughly half of the commonly used prediction, with consequences for various fields [L. Hariasz et al., companion paper, Phys. Rev. C 108, 014327 (2023)].
The muon capture reaction μ – + d → n + n + ν μ in the doublet hyperfine state is studied using nuclear potentials and consistent currents derived in the chiral effective field theory, which are local and expressed in coordinate space (the so-called Norfolk models). Only the largest contribution due to the 1 S 0 nn scattering state is considered. Particular attention is given to the estimate of theoretical uncertainty, for which four sources have been identified: 1) the model dependence, 2) the chiral-order convergence for the weak nuclear current, 3) the uncertainty in the single-nucleon axial form factor, and 4) the numerical technique adopted to solve the bound and scattering A = 2 systems. This last source of uncertainty has turned out to be essentially negligible. For the 1 S 0 doublet muon capture rate Γ D ( 1 S 0 ), we obtain Γ D ( 1 S 0 ) = 255.8(0.6) (4.4)(2.9) s –1 , where the three errors come from the first three sources of uncertainty. The value for Γ D ( 1 S 0 ) obtained within this local chiral framework is compared with previous calculations and found in very good agreement.
Potassium-40 is a widespread, naturally occurring isotope whose radioactivity impacts estimated geological ages spanning billions of years, nuclear structure theory, and subatomic rare-event searches—including those for dark matter and neutrinoless double-beta decay. The decays of this long-lived isotope must be precisely known for its use as a geochronometer, and to account for its presence in low-background experiments. There are several known decay modes for potassium-40, but a predicted electron-capture decay directly to the ground state of argon-40 has never been observed. The existence of this decay mode impacts several fields, while theoretical predictions span an order of magnitude. Here we report on the first, successful observation of this rare decay mode, obtained by the KDK (potassium decay) Collaboration using a novel combination of a low-threshold x-ray detector surrounded by a tonne-scale, high-efficiency γ -ray tagger at Oak Ridge National Laboratory. A blinded analysis reveals a distinctly nonzero ratio of intensities of ground-state electron-captures ( I EC 0 ) over excited-state ones ( I EC * ) of I EC 0 / I EC * = 0.0095 ± stat 0.0022 ± sys 0.0010 (68% CL), with the null hypothesis rejected at 4 σ [Stukel et al. , Phys. Rev. Lett. 131 , 052503 (2023) ]. In terms of branching ratio, this unambiguous signal yields I EC 0 = 0.098 % ± stat 0.023 % ± sys 0.010 % , roughly half of the commonly used prediction. This first observation of a third-forbidden unique electron capture improves our understanding of low-energy backgrounds in dark-matter searches and has implications for nuclear-structure calculations. For example, a shell-model based theoretical estimate for the neutrinoless double-beta decay half-life of calcium-48 is increased by a factor of 7 - 2 + 3 . Our nonzero measurement shifts geochronological ages by up to a percent; implications are illustrated for Earth and solar system chronologies.
Measurement of ( n,γ ) cross sections measurements are of high importance to many fields such as radiochemical diagnostics, technical nuclear forensics, nuclear physics and astrophysics, nuclear criticality safety, advanced reactors, and isotope production. For these applications an accurate characterization of the resonances in the resolved resonance region is important. In the energy range of the resonance region neutron capture, and scattering are possible so the total resonance width Γ is the sum of the gamma and neutron widths Γ = Γ γ +Γ n .
The semi-magic 110-122 Sn isotopes display signs of shape coexistence in their excited 0 + states, which, in contrast to the spherical 0+ ground states, are deformed. Here, this paper investigates the nuclear structure of 114 Sn using the competing β + decay and electron capture of a radioactive beam of 114 Sb produced at the TRIUMF-ISAC facility using the GRIFFIN spectrometer. This study will allow for an in-depth understanding of the excited 0 + states in 114 Sn, by focusing on their decay patterns. In the present experiment, transitions at 856.2-keV and 1405.0-keV, which were observed in an earlier β + decay study but not placed in the 114 Sn level scheme, have been Physics, assigned to the level scheme in connection to the 0$^+_3$ level at 2156.0-keV. Properly assigning these transitions refines the level scheme and enhances our understanding of the nuclear structure in 114 Sn.
Many advanced nuclear reactor concepts currently being developed are targeting higher operating temperatures relative to the current fleet of light water nuclear reactors, for efficiency gains and other operational considerations. The design of high temperature structural components with reliable long-term operational performance will depend on material models that accurately capture the inelastic deformation mechanisms active in these environments. In this work, we perform a detailed parameter sensitivity analysis of two unified elasto-viscoplastic Grade 91 material models capable of capturing long term high temperature creep deformation. The first model is a phenomelogical material model from the Nuclear Engineering Material Library (NEML) developed at Argonne National Lab. The NEML model parameters and their uncertainty were fit to a range of Grade 91 experimental data using Bayesian Markov Chain Monte Carlo analysis. The second model is a LAROMance data-driven surrogate material model developed at Los Alamos National Lab. The LAROMance model is fit to a large database of responses produced by a mechanistic crystal plasticity based polycrystal model. Parameters for the LAROMance surrogate material model reflect the pedigree of the Grade 91 microstructure. Both material models have been integrated into the Grizzly code, based on the open-source MOOSE multiphysics simulation framework, to simulate both the progression of aging mechanisms and the effects of that aging on nuclear power plant structures. Grizzly is used analyze a three-dimensional Grade 91 piping system to compare the long-term inelastic response predicted by these two fundamentally different models and assess the sensitivity of the material model input parameters on this quantity of interest.
Reducing CO 2 emissions from coal-fired electricity generation in China is critical to limit global warming. Long-term projections of China's electricity supply tend to assume that coal generation will be a mainstay of China's electricity system through 2050, due to limitations in the scalability of hydropower, nuclear, and natural gas generation and the commercial availability of carbon capture and storage. This paper examines the resource, economic, and institutional implications of reducing and replacing coal generation in China with mostly renewable energy and energy storage by 2040. We find that the scale of solar, wind, and storage resources needed to do so is on the order of 100–150 GW/year of solar and wind capacity and 15 GW/year of energy storage from 2020 to 2025, growing to 250 GW/year and 90 GW/year, respectively, from 2025 to 2040. We then also evaluate the sensitivities if coal plants are retired by 2050.
This dissertation is partitioned into two parts: phenomenological studies focused on rare lepton decays as probes of heavy and light new physics, and the development of differentiable, data-driven hadronization models. Part I develops the phenomenology of new physics signatures stemming from rare charged lepton flavor violating decays probed by experiments at the intensity frontier. These include interactions mediated by both high-scale effective operators and light new physics, manifesting in multi-lepton final states ($\mu \to 5e$), elastic nuclear transitions ($\mu \to e$ conversion), baryon-number-violating muon capture, and time-dependent signals from ultralight dark matter ($\mu \to e \phi, \tau \to \ell \phi$). Part II develops two distinct strategies for advancing differentiable and data-driven hadronization models. One involves comprehensive reweighting frameworks for hadronization that enable efficient uncertainty estimation, facilitate parameter tuning, and interface naturally with differentiable programming paradigms. The other introduces machine-learning-based methods for extracting microscopic fragmentation dynamics directly from macroscopic observables through the deformation of existing models -- effectively providing solutions to the inverse problem of hadronization. Altogether, these studies advance the interpretability, flexibility, and precision of theoretical predictions for both high-intensity and high-energy experiments.
Isotope harvesting is a method of collecting the long-lived radioisotopes that build up during the operation of ion-beam facilities in a way that is useful for subsequent research. As a demonstration of this method for the collection of a group IV metal at a fragmentation facility, the high-energy Zr 88 secondary beam produced from a 140-MeV/u Mo 92 primary beam at the National Superconducting Cyclotron Laboratory (NSCL) was stopped in a water target. The setup aimed to mimic the aqueous beam dump that will be implemented at the Facility for Rare Isotope Beams (FRIB). The collected Zr 88 and accompanying Y 88 decay daughter were radiochemically extracted from the solution and made into target samples suitable for neutron-capture cross-section measurements. These samples were then irradiated at two reactor facilities, and the Zr 88 average thermal-neutron-capture cross section ( σ T ) and resonance integral ( I ) were determined to be σ T = ( 8.04 ± 0.63 ) × 10 5 b and I = ( 2.53 ± 0.28 ) × 10 6 b. The σ T value agrees well with previous results and I , determined for the first time here, was found to be the largest measured resonance integral by two orders of magnitude. The Y 88 thermal-neutron-capture cross section was determined to be less than 1.8 × 10 4 b. This work demonstrates the steps needed to make cross-section measurements with samples produced via aqueous isotope harvesting.