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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Artificial Neural Networks as Mappings between Proton Potentials, Wave Functions, Densities, and Energy Levels

We report artificial neural networks (ANNs) have become important in quantum chemistry. Herein, applications to nuclear quantum effects, such as zero-point energy, vibrationally excited states, and hydrogen tunneling, are explored. ANNs are used to solve the time-independent Schrödinger equation for single- and double-well potentials representing hydrogen-bonded molecular systems capable of proton transfer. ANN mappings are trained to predict the lowest five proton vibrational energies, wave functions, and densities from the proton potentials and to predict the excited state proton vibrational energies and densities from the proton ground state density. For the inverse problem, ANN mappings are trained to predict the proton potential from the proton vibrational energy levels or the proton ground state density. This latter mapping is theoretically justified by the first Hohenberg-Kohn theorem establishing a one-to-one correspondence between the external potential and the ground state density. ANNs for two- and three-dimensional systems are also presented to illustrate the straightforward extension to higher dimensions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Multimodal fission from self-consistent calculations

When multiple fission modes coexist in a given nucleus, distinct fragment yield distributions appear. Multimodal fission has been observed in a number of fissioning nuclei spanning the nuclear chart, and this phenomenon is expected to affect the nuclear abundances synthesized during the rapid neutron-capture process (𝑟-process). In this study, we generalize the previously proposed hybrid model for fission-fragment yield distributions to predict competing fission modes and estimate the resulting yield distributions. Here, our framework allows for a comprehensive large-scale calculation of fission-fragment yields suited for 𝑟-process nuclear network studies. Nuclear density functional theory is employed to obtain the potential energy and collective inertia tensor on a multidimensional collective space defined by mass multipole moments. Fission pathways and their relative probabilities are determined using the nudged elastic band method. Based on this information, mass and charge fission yields are predicted using the recently developed hybrid model. Fission properties of fermium isotopes are calculated in the axial quadrupole-octupole collective space for three energy density functionals (EDFs). Disagreement between the EDFs appears when multiple fission modes are present. Within our framework, the UNEDF⁢1 HFB EDF agrees best with experimental data. Calculations in the axial quadrupole-octupole-hexadecapole collective space improve the agreement with the experiment for SkM*. We also discuss the sensitivity of fission predictions on the choice of EDF for several superheavy nuclei. Fission-fragment yield predictions for nuclei with multiple fission modes are sensitive to the underlying EDF. For large-scale calculations in which a minimal number of collective coordinates is considered, UNEDF⁢1 HFB provides the best description of experimental data, though the sensitivity motivates robust quantification of the uncertainties of the theoretical model.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Landscape of pear-shaped even-even nuclei

The phenomenon of reflection-asymmetric nuclear shapes is relevant to nuclear stability, nuclear spectroscopy, nuclear decays and fission, and the search for new physics beyond the standard model. Global surveys of ground-state octupole deformation, performed with a limited number of models, suggest that the number of pear-shaped isotopes is fairly limited across the nuclear landscape. Here, we carry out a global analysis of ground-state octupole deformations for particle-bound even-even nuclei with Z ≤ 110 and N ≤ 210 using nuclear density functional theory (DFT) with several nonrelativistic and covariant energy density functionals. In this way, we can identify the best candidates for reflection-asymmetric shapes. The calculations are performed in the frameworks of axial reflection-asymmetric Hartree-Fock-Bogoliubov theory and relativistic Hartree-Bogoliubov theory using DFT solvers employing harmonic oscillator basis expansion. We consider five Skyrme and four covariant energy density functionals. We predict several regions of ground-state octupole deformation. In addition to the “traditional” regions of neutron-deficient actinide nuclei around 224 Ra and neutron-rich lanthanides around 146 Ba, we identified vast regions of reflection-asymmetric shapes in very neutron-rich nuclei around 200 Gd and 288 Pu, as well as in several nuclei around 112 Ba. Our analysis suggests several promising candidates with stable ground-state octupole deformation, primarily in the neutron-deficient actinide region, that can be reached experimentally. Detailed comparison between Skyrme and covariant models is performed. Octupole shapes predicted in this study are consistent with the current experimental information. This work can serve as the starting point of a systematic search for parity doublets in odd-mass and odd-odd nuclei, which will be of interest in the context of new physics searches.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

Fast Emulation of Expensive Simulations using Approximate Gaussian Processes [Slides]

Nuclear Computational Low-Energy Initiative (NUCLEI) collaboration uses Density Functional Theory (DFT) simulations to predict the structure and binding energies of nuclei over a wide range of proton (Z) and neutron (N) numbers. The DFT simulations utilize a particular parameterization of a Skyrme energy density functional called UNEDF1 which depends on 12 free parameters that must be fit to data (M Kortelainen et al 2014). Fitting involves comparing (e.g.) predicted binding energies of nuclei to experimentally measured values. We use only binding energies as observables, but DFT with UNEDF1 will predict structure (shape) observables as well. In this work, assessing the capability of approximate GP emulators to balance emulator accuracy with computational speed to facilitate improved UNEDF1 calibration. Sparse GPs are straightforward to train and accurate. Calibration is not straightforward with MCMC (using MH or HMC/NUTS). We produced reusable software for continuing and building on this work as well as accessing and using Darwin cluster compute resources

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2020

Primary $\gamma$-ray intensities and $\gamma$-strength functions from discrete two-step $\gamma$-ray cascades in radiative proton-capture experiments

Background: Reaction rates of radiative capture reactions can play a crucial role in the nucleosynthesis of heavy nuclei in explosive stellar environments. These reaction rates depend strongly on $\gamma$-ray decay widths in the reaction products, which are, for nonresonant capture reactions at high excitation energies, derived from the $\gamma$-ray strength function and the nuclear level density. Recently, the ratio method was applied to primary $\gamma$ rays observed from ($\textit{d, p}$) reactions and nuclear resonance fluorescence measurements to extract the dipole strength in atomic nuclei and to test the generalized Brink-Axel hypothesis. Purpose: The purpose of this work is to apply the ratio method to primary $\gamma$-ray intensities of the 63,65 Cu($\textit{p},\gamma$) reactions to extract $\gamma$-ray strength information on the nuclei 64,66 Zn. Here, the impact of spin distribution, total $\gamma$-ray decay widths, level densities, and width fluctuations on the application of the ratio method will be discussed. Additionally, by comparing the relative $\gamma$-ray strength at different excitation energies, conclusions on the validity of the generalized Brink-Axel hypothesis can be made. Method: The radiative proton capture reaction measurements have been performed at the HORUS $\gamma$-ray spectrometer of the University of Cologne at one excitation energy for each reaction. Primary $\gamma$-ray intensities have been determined by normalizing secondary $\gamma$-ray transitions in two-step cascades using their absolute branching ratio. The ratio method was applied to the measured primary $\gamma$-ray intensities as well as to previous measurements by Erlandsson et al. at different excitation energies. Results: The relative strength function curve for 64 Zn from our measurement shows no significant deviation from the previous measurement at a different excitation energy. The same is true for 66 Zn where both measurements were at almost the same excitation energy. Absolute $\gamma$-strength function values have been obtained by normalizing the relative curves to quasiparticle random phase approximation calculations because of the absence of experimental data in the respective energy region. Conclusion: The generalized Brink-Axel hypothesis, i.e., the independence of the strength function on the excitation energy, seems to hold in the studied energy region and nuclei. The method to obtain primary $\gamma$-ray intensities from two-step cascade spectra was shown to be a valuable and sensitive tool although its uncertainties are connected to the knowledge of the low-energy level scheme of the investigated nucleus. The scaling in the ratio method should be taken with care, because the relative strength is not a simple sum of $f_{E1}$ and $f_{M1}$ but a somewhat complex linear combination dependent on the excitation energy of the nucleus.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Electronic Structures and Magnetism of Zr-, Th-, and U-based Metal-Organic Frameworks (MOFs) by Density Functional Theory

Metal-organic frameworks (MOFs) have recently gained wide interest as candidate materials for nuclear waste immobilization. While the fundamental thermodynamic properties, such as the substitution energies determine the favorability of radionuclide sequestration by utilization of a MOF matrix, the studies of MOF electronic structure reveal the role of d-, and/or f-electrons on changes in physical properties of actinide-containing materials. We use density functional theory (DFT) calculations to investigate the electronic structures of Zr-, Th-, and U-MOFs, including their electronic band structures and, where appropriate, their magnetic properties. We employ various DFT methods including DFT+U, collinear spin-polarization, spin-orbit coupling, and different flavors of exchange-correlation functionals to assess the robustness to the specific exchange-correlation functional. Unlike the Zr-, and Th-MOFs, the U-MOF is found to be sensitive to electron localization and spin; hence we explore the magnetic structure of the U-MOF in further detail.

Metal-Organic Framework, MOF, Actinides, DFT↗
DOE OSTI2026

Neutron skins probed in proton knockout from neutron-rich nuclei

Proton-induced quasifree knockout reactions provide a powerful probe of nuclear single-particle structure and reaction dynamics in both stable and neutron-rich nuclei. Here, in this work, we develop a unified theoretical framework for the calculation of inclusive (𝑝, 2⁢𝑝) and sequential (𝑝, 3⁢𝑝) reaction cross sections and fragment momentum distributions at intermediate and relativistic energies. The approach is based on a probabilistic extension of Glauber multiple-scattering theory combined with microscopic nuclear densities obtained from Hartree-Fock-Bogoliubov calculations using Skyrme energy-density functionals. We focus in particular on the sensitivity of total cross sections and longitudinal momentum dispersions to neutron-skin thickness along isotopic chains. Our results indicate that both (𝑝, 2⁢𝑝) and (𝑝, 3⁢𝑝) reactions exhibit a systematic decrease of cross section and momentum width with increasing neutron excess, reflecting enhanced attenuation and surface bias induced by neutron skins. The effect is significantly stronger for two-proton removal, suggesting that (𝑝, 3⁢𝑝) reactions may offer enhanced sensitivity to isovector nuclear structure. These findings establish proton-induced knockout reactions as complementary hadronic probes of neutron skins and the density dependence of the nuclear symmetry energy.

direct reactions↗
DOE OSTI2020

Elucidation of Bottom-up Growth of CaCO3 Involving Prenucleation Clusters from Structure Predictions and Decomposition of Globally Optimized (CaCO3)n Nanoclusters

Low-energy minima structures for (CaCO3)n, n = 28, are predicted using bottom-up genetic algorithms in conjunction with density functional theory electronic structure calculations, in comparison with the frozen and relaxed top-down clusters generated by cuts from the calcite, vaterite, and aragonite crystal structures. Similarities in structural motifs for the bottom-up and relaxed top-down are revealed using a fragment recognition technique. Fragment energy decomposition analysis shows that the bottom-up and relaxed top-down clusters belong to two classes of amorphous clusters with distinct intracluster energy distributions, despite their structural similarity. The bottom-up clusters with >20 formula units are surface stabilized with negative surface energy densities. In contrast, the top-down clusters are interior stabilized with positive surface energy densities. We prove that the sign of the surface energy density determines whether the nucleation reaction energy as a function of nuclear size has a maximum or a minimum. The surface-stabilized bottom-up clusters are proposed to be a type of prenucleation cluster at the minimum of the nucleation reaction energy. A mechanism for mineralization of CaCO3 involving prenucleation clusters and nonclassical growth pathway is proposed on the basis of our theoretical findings, which is consistent with previous titration experiments.

calcium carbonate, prenucleation cluster, biominer↗
DOE OSTI2022

Estimates of Quantum Tunneling Effects for Hydrogen Diffusion in PuO 2

We detail the estimation of activation energies and quantum nuclear vibrational tunneling effects for hydrogen diffusion in PuO 2 based on Density Functional Theory calculations and a quantum double well approximation. We find that results are relatively insensitive to choice of exchange correlation functional. In addition, the representation of spin in the system and use of an extended Hubbard U correction has only a small effect on hydrogen point defect formation energies when the PuO 2 lattice is held fixed at the experimental density. We then compute approximate activation energies for transitions between hydrogen interstitial sites seeded by a semi-empirical quantum model and determine the quantum tunneling enhancement relative to classical kinetic rates. Our model indicates that diffusion rates in H/PuO 2 systems could be enhanced by more than one order of magnitude at ambient conditions and that these effects persist at high temperature. The method we propose here can be used as a fast screening tool for assessing possible quantum nuclear vibrational effects in any number of condensed phase materials and surfaces, where hydrogen hopping tends to follow well defined minimum energy pathways.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Investigating effects of relativistic kinematics, dimensionality, interactions, and short-range correlations on the ratio of quartic over quadratic nuclear symmetry energies

While ample evidence for the so-called empirical parabolic law of the Equation of State (EOS) of isospin asymmetric nuclear matter (ANM) has been obtained in many studies within both non-relativistic and relativistic nuclear many-body theories using various interactions, it has been unclear if there is any fundamental physics reason for the small quartic symmetry energy compared to the quadratic one even as the ANM approaches pure neutron matter. Within both relativistic and non-relativistic Free Fermi Gas (FFG) models in coordinate spaces of arbitrary dimension d with and without considering Short-Range Correlations (SRC) as well as non-linear Relativistic Mean Field (RMF) models, we study effects of relativistic kinematics, dimensionality, interactions and SRC on the ratio Ψ(ρ) of quartic over quadratic symmetry energies in ANM EOSs. We found that the ratio Ψ(ρ) in the FFG model depends strongly on the dimension d. While it is very small already in the normal 3D space, it could be even smaller in spaces with reduced dimensions for sub-systems of particles in heavy-ion reactions and/or whole neutron stars due to constraints, collectivities and/or symmetries. Here, we also found that the ratio Ψ(ρ) could theoretically become very large only at the ultra-relativistic limit far above the density reachable in neutron stars. On the other hand, nuclear interaction directly and/or indirectly through SRC-induced high-momentum nucleons affect significantly the density dependence of Ψ(ρ) compared to the relativistic FFG model prediction. The SRC affects significantly not only the kinetic energy of symmetric nuclear matter but also the ratio Ψ(ρ) while the relativistic corrections are found negligible. The results may help better understand the EOS of dense neutron-rich matter.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Theoretical uncertainty quantification for heavy-ion fusion

Despite recent advances and focus on rigorous uncertainty quantification for microscopic models of quantum many-body systems, the uncertainty on the dynamics of those systems has been underexplored. To address this, we have used time-dependent Hartree-Fock to examine the model uncertainty for a collection of low-energy, heavy-ion fusion reactions. Fusion reactions at near-barrier energies represent a rich test-bed for the dynamics of quantum many-body systems owing to the complex interplay of collective excitation, transfer, and static effects that determine the fusion probability of a given system. The model uncertainty is sizable for many of the systems studied and the primary contribution arises from static properties that are ill-constrained, such as the neutron radius of neutron-rich nuclei. Furthermore, these large uncertainties motivate the use of information from reactions to better constrain existing models and to infer static properties from reaction data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Precision Determination of the Neutral Weak Form Factor of Ca 48

In this work, we report a precise measurement of the parity-violating asymmetry $A_{\rm PV}$ in the elastic scattering of longitudinally polarized electrons from $^{48}{\rm Ca}$. We measure $A_{\rm PV} =2668\pm 106\ {\rm (stat)}\pm 40\ {\rm (syst)}$ parts per billion, leading to an extraction of the neutral weak form factor $F_{\rm W} (q=0.8733$ fm$^{-1}) = 0.1304 \pm 0.0052 \ {\rm (stat)}\pm 0.0020\ {\rm (syst)}$ and the charge minus the weak form factor $F_{\rm ch} - F_{\rm W} = 0.0277\pm 0.0055$. The resulting neutron skin thickness $R_n-R_p=0.121 \pm 0.026\ {\rm (exp)} \pm 0.024\ {\rm (model)}$~fm is relatively thin yet consistent with many model calculations. The combined CREX and PREX results will have implications for future energy density functional calculations and on the density dependence of the symmetry energy of nuclear matter.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

First Measurement of the Neutron-Emission Probability with a Surrogate Reaction in Inverse Kinematics at a Heavy-Ion Storage Ring

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.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Accelerating multiscale electronic stopping power predictions with time-dependent density functional theory and machine learning

Knowing the rate at which particle radiation releases energy in a material, the “stopping power,” is key to designing nuclear reactors, medical treatments, semiconductor and quantum materials, and many other technologies. While the nuclear contribution to stopping power, i.e., elastic scattering between atoms, is well understood in the literature, the route for gathering data on the electronic contribution has for decades remained costly and reliant on many simplifying assumptions, including that materials are isotropic. We establish a method that combines time-dependent density functional theory (TDDFT) and machine learning to reduce the time to assess new materials to hours on a supercomputer and provide valuable data on how atomic details influence electronic stopping. Our approach uses TDDFT to compute the electronic stopping from first principles in several directions and then machine learning to interpolate to other directions at a cost of 10 million times fewer core-hours. We demonstrate the combined approach in a study of proton irradiation in aluminum and employ it to predict how the depth of maximum energy deposition, the “Bragg Peak,” varies depending on the incident angle—a quantity otherwise inaccessible to modelers and far outside the scales of quantum mechanical simulations. The lack of any experimental information requirement makes our method applicable to most materials, and its speed makes it a prime candidate for enabling quantum-to-continuum models of radiation damage. The prospect of reusing valuable TDDFT data for training the model makes our approach appealing for applications in the age of materials data science.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Analytic Nuclear Gradients for Complete Active Space Linearized Pair-Density Functional Theory

Accurately modeling photochemical reactions is difficult due to the presence of conical intersections and locally avoided crossings, as well as the inherently multiconfigurational character of excited states. As such, one needs a multistate method that incorporates state interaction in order to accurately model the potential energy surface at all nuclear coordinates. The recently developed linearized pair-density functional theory (L-PDFT) is a multistate extension of multiconfiguration PDFT, and it has been shown to be a cost-effective post-MCSCF method (as compared to more traditional and expensive multireference many-body perturbation methods or multireference configuration interaction methods) that can accurately model potential energy surfaces in regions of strong nuclear–electronic coupling in addition to accurately predicting Franck–Condon vertical excitations. Here, in this paper, we report the derivation of analytic gradients for L-PDFT and their implementation in the PySCF-forge software, and we illustrate the utility of these gradients for predicting ground- and excited-state equilibrium geometries and adiabatic excitation energies for formaldehyde, s-trans-butadiene, phenol, and cytosine.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Information Content of the Parity-Violating Asymmetry in Pb 208

The parity-violating asymmetry A PV in 208 Pb, recently measured by the PREX-2 Collaboration, is studied using modern relativistic (covariant) and nonrelativistic energy density functionals. We first assess the theoretical uncertainty on A PV which is intrinsic to the adopted approach. To this end, we use quantified functionals that are able to accommodate our previous knowledge on nuclear observables such as binding energies, charge radii, and the dipole polarizability α D of 208 Pb. We then add the quantified value of A PV together with α D to our calibration dataset to optimize new functionals. Based on these results, we predict a neutron skin thickness in 208 Pb r skin = 0.19 ± 0.02 fm and the symmetry-energy slope L = 54 ± 8 MeV. These values are consistent with other estimates based on astrophysical data and are significantly lower than those recently reported using a particular set of relativistic energy density functionals. Here, we also make a prediction for the A PV value in 48 Ca that will be soon available from the CREX measurement.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2026

Mass of 101 Sn and Bayesian extrapolations to the proton drip line

The favorable energy configurations of nuclei at magic numbers of 𝑁 neutrons and 𝑍 protons are fundamental for understanding the evolution of nuclear structure. The 𝑍 = 50 (tin) isotopic chain is a frontier for such studies, with particular interest at and around the doubly magic 100 Sn isotope, for which the mass is a topic of debate. Precise mass values for neutron-deficient isotopes provide necessary anchor points for mass models to test extrapolations near the proton drip line, where experimental studies remain out of reach. In this work, we report a Penning trap mass measurement of 101 Sn . The determined mass excess of −59889.89⁢(96) keV for 101 Sn represents a factor-of-300 improvement over the current precision and indicates that 101 Sn is less bound than previously thought. Mass predictions from a recently developed Bayesian model combination framework employing statistical machine learning and nuclear masses computed within seven global models based on nuclear density functional theory agree within 1⁢𝜎 with experimental masses from the 48 ≤ 𝑍 ≤ 52 isotopic chains. The framework's resilience to new mass data gave confidence in the extrapolation of tin masses down to 𝑁 = 46. Our calculations suggest that 96 Sn is a two-proton drip line nucleus and predict a mass excess of −58090⁢(800) keV for 100 Sn , showing a preference within 1⁢𝜎 for the mass of 100 Sn derived from the 𝛽-delayed 𝑄 value measured at GSI.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗