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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 1,441 records · Page 80

Variationally consistent approximation scheme for charge transfer

The author has developed a technique for testing various charge-transfer approximation schemes for consistency with the requirements of the Kohn variational principle for the amplitude to guarantee that the amplitude is correct to second order in the scattering wave functions. Applied to Born-type approximations for charge transfer it allows the selection of particular groups of first-, second-, and higher-Born-type terms that obey the consistency requirement, and hence yield more reliable approximation to the amplitude.

Halpern, A. M.↗

The anisotropic radiative transfer problem in optically thick, strongly magnetized plasma - A comparison of results

The accuracy of four different methods for solving the coherent radiative transfer problem in a strongly magnetized plasma is compared. Specific attention is given to the case of a semi-infinite homogeneous plasma with a magnetic field perpendicular to the surface. The four approaches evaluated were: diffusion approximation schemes; the generalized H-function method of Silant'ev (1982) the Feautrier method of Nagel (1981) and the integral equation approach of Meszares and Bonazzola (1981). It is found that the coupled diffusion approximation schemes of Nagel (1981) and Kaminker et al. (1982) provided satisfactory results and were more efficient in many cases than direct numerical methods.

Pavlov, G. G.↗

A Posteriori Error Estimation for Discontinuous Galerkin Approximations of Hyperbolic Systems

This article considers a posteriori error estimation of specified functionals for first-order systems of conservation laws discretized using the discontinuous Galerkin (DG) finite element method. Using duality techniques, we derive exact error representation formulas for both linear and nonlinear functionals given an associated bilinear or nonlinear variational form. Weighted residual approximations of the exact error representation formula are then proposed and numerically evaluated for Ringleb flow, an exact solution of the 2-D Euler equations.

Larson, Mats G.↗

Inversion and approximation of Laplace transforms

A method of inverting Laplace transforms by using a set of orthonormal functions is reported. As a byproduct of the inversion, approximation of complicated Laplace transforms by a transform with a series of simple poles along the left half plane real axis is shown. The inversion and approximation process is simple enough to be put on a programmable hand calculator.

Lear, W. M.↗

First-Principles Study of Pressure Dependence of Optical Spectra of MnS

MnS is a semiconductor material that can be used in solar cell coatings as window/buffer material and in many other applications. The present contribution deals with the optical properties of MnS in the zinc-blende structure using ab initio calculations within the generalized gradient approximation. Features such as dielectric function, refractive index, reflectivity, optical absorption, conductivity, and electron loss function spectra have been reported and their pressure dependence has been examined and discussed. The information gathered from the present study can be useful for photovoltaic applications.

14 SOLAR ENERGY↗

Structural, Elastic, Thermodynamic, Electronic, and Magnetic Investigations of Full-Heusler Compound Ag{sub 2}CeAl: FP-LAPW Method

Structural, elastic, thermodynamic, electronic, and magnetic properties of the full-Heusler compound Ag{sub 2}CeAl were determined using generalized gradient approximation with exchange-correlation functional GGA (PBEsol) with spin-orbit coupling (SOC) correction. The elastic modulus and their pressure dependence are calculated. From the elastic parameter behavior, it is inferred that this compound is elastically stable and ductile in nature. Through the quasi-harmonic Debye model, in which the phononic effect is considered the effect of pressure P (0 to 50) and temperature T (0 to 1000) on the lattice constant, the elastic parameters, bulk modulus B, heat capacity and thermal expansion α, internal energy U, entropy S, Debye temperature 𝜃{sub D}, Helmholtz free energy A, and Gibbs free energy G are investigated. The thermodynamic properties show that the compound Ag{sub 2}CeAl is a heavy fermion material. The density of state (DOS), magnetic momentum, and band structure are computed, to investigate the magnetic and metallic characteristics. The calculated polarization of the compound is 77.34%. The obtained results are the first predictions of the physical properties for the rare-earth-based (Ce) full-Heusler Ag{sub 2}CeAl.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Thermo-hydraulic steam pipe models for district heating simulations: Simplifications to balance accuracy and simulation speed

Steam piping networks are essential for optimizing performance in industrial processes and district heating systems. However, dynamic models that balance thermo-hydraulic accuracy with computational efficiency remain limited. In response, this paper presents a new discretized steam pipe model based on the plug flow approach, capturing key thermo-hydraulic behaviors while simplifying steam phase change processes. Implemented in Modelica, the model accurately calculates temperature and pressure distributions along steam pipelines. To improve computational efficiency for district-scale simulations, five model simplifications are introduced: lumped thermo-hydraulic functions, empirical correlations, fluid state approximations, steady-state dynamics and inclusion of flow derivatives. These simplified models achieve 85%-98% accuracy in predicting pressure drop and condensation losses, including dynamic condensate behavior during pipe warm-up—a factor often overlooked in existing models. The models support diverse network configurations, scaling effectively to systems with multiple distribution pipes and connected building loads. Discrete models provide detailed insights but exhibit a cubic increase in simulation time as the network scales by N connected building O(N 2.42 ). In contrast, lumped models simulate 10–28 times faster than discrete, offering quadratic scaling of simulation time O(N 1.73 ). However, they still require 6 times more computation time than a lossless network, highlighting the inherent computational challenges of modeling compressible fluid flow. In conclusion, the steady-state lumped variant, with its near-linear scalability in computational time O(N 1.01 ), emerges as an efficient solution for preliminary design evaluations and extensive parametric studies.

15 GEOTHERMAL ENERGY↗

Partitioned exponential methods for coupled multiphysics systems

Multiphysics problems involving two or more coupled physical phenomena are ubiquitous in science and engineering. This work develops a new partitioned exponential approach for the time integration of multiphysics problems. After a possible semi-discretization in space, the class of problems under consideration is modeled by a system of ordinary differential equations where the right-hand side is a summation of two component functions, each corresponding to a given set of physical processes. The partitioned-exponential methods proposed herein evolve each component of the system via an exponential integrator, and information between partitions is exchanged via coupling terms. Here, the traditional approach to constructing exponential methods, based on the variation-of-constants formula, is not directly applicable to partitioned systems. Rather, our approach to developing new partitioned-exponential families is based on a general-structure additive formulation of the schemes. Two method formulations are considered, one based on a linear-nonlinear splitting of the right hand component functions, and another based on approximate Jacobians. The paper develops classical (non-stiff) order conditions theory for partitioned exponential schemes based on particular families of T-trees and B-series theory. Several practical methods of third order are constructed that extend the Rosenbrock-type and EPIRK families of exponential integrators. Several implementation optimizations specific to the application of these methods to reaction-diffusion systems are also discussed. Numerical experiments reveal that the new partitioned-exponential methods can perform better than traditional unpartitioned exponential methods on some problems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Compressed sparse tensor based quadrature for vibrational quantum mechanics integrals

A new method for fast evaluation of high dimensional integrals arising in quantum mechanics is proposed. Here, the method is based on sparse approximation of a high dimensional function followed by a low-rank compression. In the first step, we interpret the high dimensional integrand as a tensor in a suitable tensor product space and determine its entries by a compressed sensing based algorithm using only a few function evaluations. Secondly, we implement a rank reduction strategy to compress this tensor in a suitable low-rank tensor format using standard tensor compression tools. This allows representing a high dimensional integrand function as a small sum of products of low dimensional functions. Finally, a low dimensional Gauss–Hermite quadrature rule is used to integrate this low-rank representation, thus alleviating the curse of dimensionality. Finally, numerical tests on synthetic functions, as well as on energy correction integrals for water and formaldehyde molecules demonstrate the efficiency of this method using very few function evaluations as compared to other integration strategies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Reproducibility in G 0 W 0 calculations for solids

Ab initio many-body perturbation theory within the GW approximation is a Green's function formalism widely used in the calculation of quasiparticle excitation energies of solids. In what has become an increasingly standard approach, Kohn–Sham eigenenergies, generated from a DFT calculation with a strategically-chosen exchange–correlation functional “starting point”, are used to construct G and W, and then perturbatively corrected by the resultant GW self-energy. In practice, there are several ways to construct the GW self-energy, and these can lead to variations in predicted quasiparticle energies. For example, for ZnO and TiO 2 , the GW fundamental gaps reported in the literature can vary by more than 1 eV depending on the GW code used. In this work, we calculate and analyze GW quasiparticle (QP) energies of these and other systems with three different GW codes: BERKELEYGW, ABINIT and YAMBO. Through a systematic analysis of the GW implementation of these three codes, we identify the primary origin of major discrepancies between codes reported in prior literature to be the different implementations the Coulomb divergence in the Fock exchange term and the frequency integration scheme of the GW self-energy. We then eliminate these discrepancies by using common numerical methods and algorithms, demonstrating that the same quasiparticle energies for a given material can be obtained with different codes, within numerical differences ascribable to the technical details of the underling implementations. This work will be important for users and developers in assessing the precision of future GW applications and methods.

36 MATERIALS SCIENCE↗

Physics-constrained deep neural network method for estimating parameters in a redox flow battery

Here, in this paper, we present a physics-constrained deep neural network (PCDNN) method for parameter estimation in the zero-dimensional (0D) model of the vanadium redox flow battery (VRFB). In this approach, we use deep neural networks to approximate the model parameters as functions of the operating conditions. This method allows the integration of VRFB computational models as the physical constraints in the parameter learning process, leading to enhanced accuracy of parameter estimation and cell voltage prediction. Using an experimental dataset, we demonstrate that the PCDNN method can estimate model parameters for a range of operating conditions and improve the 0D model prediction of voltage compared to the 0D model prediction with constant operation-condition-independent parameters estimated with traditional inverse methods. We also demonstrate that the PCDNN approach has an improved generalization ability for estimating parameter values for operating conditions not used in the training process.

25 ENERGY STORAGE↗

A flexible event reconstruction based on machine learning and likelihood principles

Event reconstruction is a central step in many particle physics experiments, turning detector observables into parameter estimates; for example estimating the energy of an interaction given the sensor readout of a detector. A corresponding likelihood function is often intractable, and approximations need to be constructed. Here, in our work, we first show how the full likelihood for a many-sensor detector can be broken apart into smaller terms, and secondly how we can train neural networks to approximate all terms solely based on forward simulation. Our technique results in a fast, flexible, and close-to-optimal surrogate model proportional to the likelihood and can be used in conjunction with standard inference techniques allowing for a consistent treatment of uncertainties. We illustrate our technique for parameter inference in neutrino telescopes based on maximum likelihood and Bayesian posterior sampling. Given its great flexibility, we also showcase our method for geometry optimization enabling to learn optimal detector designs. Lastly, we apply our method to realistic simulation of a ton-scale water-based liquid scintillator detector.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Redox Defect Thermochemistry of FeAl 2 O 4 Hercynite in Water Splitting from First-Principles Methods

Solar thermochemical hydrogen (STCH) production is a promising route to produce fuels from sunlight via high-temperature water splitting. However, efficient and technologically viable implementations of this process only allow a narrow window of thermodynamic boundary conditions that can be used to cycle the system, thus limiting the design space for suitable metal oxide redox mediators. An oxygen defect redox mechanism can contribute a favorable reduction entropy to expand this window, and computational evaluation of materials with high oxygen defect entropies could play a pivotal role in guiding the discovery and design of suitable oxides. This study employs first-principles calculations to investigate the redox mediating defect mechanism of the STCH candidate material, hercynite (FeAl 2 O 4 ). We compare the results of total energy calculations from density functional theory (DFT) with beyond-DFT approaches, including hybrid functionals and the random phase approximation, which are among the most advanced methods currently feasible for supercell defect calculations. Using the predicted formation energies, we perform thermodynamic modeling of FeAl2O4 reduction and oxidation via free energy minimization that incorporates ideal gas, configurational, and vibrational entropy contributions evaluated within the quasi-harmonic approximation. Special attention is devoted to understanding interactions among co-existing defects, such as the association of pairs and complexes of O vacancies and cation antisite defects, and the effect of mutually compensating defect charges. Our results corroborate the notion that the details of defect interactions can be decisive for the viability of hydrogen production within the desirable STCH process window.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DONKEY: A Flexible and Accurate Algorithm for Clustering

We propose an accurate clustering algorithm suitable for the varied and multidimensional data sets that correspond to temporal snapshots from on-the-fly nonadiabatic trajectory-based simulations of photoexcited dynamics. The algorithm approximates the underlying probability density function using variable kernel density estimation, with local maxima corresponding to cluster centers. Each data point is then assigned to one of the maxima by employing a maximization procedure. Finally, clusters artificially separated by minor fluctuations in the probability density are merged. The algorithm does not require parameter tuning, which ensures flexibility and reduces the risk of bias. It is tested on several synthetic data sets, where it consistently outperforms conventional clustering algorithms. As a final example, the algorithm is applied to the excited dynamics of the norbornadiene ⇌ quadricyclane (C 7 H 8 ) molecular photoswitch, demonstrating how distinct reaction pathways can be identified.

algorithms↗

Electronic Excitations in Complex Molecular Environments: Many-Body Green’s Functions Theory in VOTCA-XTP

Many-body Green’s functions theory within the GW approximation and the Bethe-Salpeter Equation (BSE) is implemented in the open-source VOTCA-XTP software, aiming at the calculation of electronically excited states in complex molecular environments. Based on Gaussian-type atomic orbitals and making use of resolution of identity techniques, the code is designed specifically for nonperiodic systems. Application to a small molecule reference set successfully validates the methodology and its implementation for a variety of excitation types covering an energy range from 2 to 8 eV in single molecules. Further, embedding each GW-BSE calculation into an atomistically resolved surrounding, typically obtained from Molecular Dynamics, accounts for effects originating from local fields and polarization. Using aqueous DNA as a prototypical system, different levels of electrostatic coupling between the regions in this GW-BSE/MM setup are demonstrated. Particular attention is paid to charge-transfer (CT) excitations in adenine base pairs. It is found that their energy is extremely sensitive to the specific environment and to polarization effects. The calculated redshift of the CT excitation energy compared to a nucelobase dimer treated in vacuum is of the order of 1 eV, which matches expectations from experimental data. Predicted lowest CT energies are below that of a single nucleobase excitation, indicating the possibility of an initial (fast) decay of such an UV excited state into a binucleobase CT exciton. Furthermore, the results show that VOTCA-XTP’s GW-BSE/MM is a powerful tool to study a wide range of types of electronic excitations in complex molecular environments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Curated Collection of More than 20,000 Experimentally Reported One-Dimensional Metal–Organic Frameworks

Herein, a collection of more than 20,000 experimentally derived crystal structures for metal–organic frameworks (MOFs) that do not have two- or three-dimensional covalently bonded networks has been developed from the materials available at the Cambridge Crystallographic Data Centre. Of these 20,000 1D MOFs, more than 12,000 structures have been verified to be solvent-free and in exact agreement with the stoichiometry of the synthesized materials. More than 10% of the complete data set comprise materials including two or more distinct metals. The band gaps of more than 12,000 1D MOFs have been computed at the density functional theory-generalized gradient approximation level, finding more than 2000 materials that have a zero band gap. Molecular simulations of CH4 adsorption in a small number of 1D MOFs indicated that adsorbate-induced deformation plays a significant role in determining adsorption isotherms in these materials. As a result, methods that have been used previously for high-throughput predictions of molecular adsorption in 3D MOFs are not suitable for 1D MOFs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Chemical Durability and Dissolution Kinetics of Iodoapatite in Aqueous Solutions

Understanding the long-term release of radionuclides from nuclear waste to the environment is critical for public acceptance and sustainability of nuclear energy. Iodoapatite, a synthetic material similar to mineral vanadinite proposed for radioactive iodine-129 immobilization, is employed in this study as a model system for iodine waste forms and ceramic waste forms in general to understand its long-term chemical durability. Semidynamic leaching experiments were performed in cap-sealed Teflon vessels to evaluate the chemical durability at temperatures from 20 to 90 degrees C and pH values from 4 to 9 using deionized water and pH buffer solutions. The leachates were analyzed using inductively coupled plasma-mass spectrometry. The leached surfaces were examined by X-ray diffraction, scanning electron microscopy, and Raman spectroscopy. Effects of test variables including surface-to-volume ratio, leachant replacement interval, and environmental variables including temperature and pH on the dissolution rate were systematically investigated. The activation energy of the dissolution was 16.9 ± 1.5 kJ/mol for the matrix elements and 34.4 ± 3.9 kJ/mol for the diffusive iodine release. The order of the pH effect on the dissolution rate as a power law exponent was 0.87 ± 0.08. The effect of the surface-to-volume ratio and replacement interval was approximated by a single exponential function rise to maximum. Fully parametrized models were then combined to predict iodine release rate under various conditions. The result suggests that the long-term iodine release is controlled by iodide diffusion when the matrix dissolution rate is very low in near neutral pH solutions and by matrix dissolution when the dissolution rate is high at low pH. The present study demonstrates a mechanistic approach to parametrize models that can be used to evaluate the performance of nuclear waste forms under various disposal environments.

36 MATERIALS SCIENCE↗

Engineering Robust Metallic Zero-Mode States in Olympicene Graphene Nanoribbons

Metallic graphene nanoribbons (GNRs) represent a critical component in the toolbox of low-dimensional functional materials technology serving as 1D interconnects capable of both electronic and quantum information transport. The structural constraints imposed by on-surface bottom-up GNR synthesis protocols along with the limited control over orientation and sequence of asymmetric monomer building blocks during the radical step-growth polymerization have plagued the design and assembly of metallic GNRs. Here, we report the regioregular synthesis of GNRs hosting robust metallic states by embedding a symmetric zero-mode (ZM) superlattice along the backbone of a GNR. Tight-binding electronic structure models predict a strong nearest-neighbor electron hopping interaction between adjacent ZM states, resulting in a dispersive metallic band. First-principles density functional theory-local density approximation calculations confirm this prediction, and the robust, metallic ZM band of olympicene GNRs is experimentally corroborated by scanning tunneling spectroscopy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗