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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 415 records · Page 23
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

NbTi_BCC_SolidSolution_128atoms_VASP6

We performed density functional theory (DFT) calculations for body-centered-cubic (BCC) structures with 128 lattices sites of solid solution binary alloys niobium-titanium (Nb-Ti). The electronic structures of alloys have been calculated using Vienna Ab initio Simulation Package (VASP), https://github.com/ORNL/ScalableWorkflow_VASP_Calculations. Within this package the DFT approach is used to reduce many-body Schrodinger equation to set of single particle Kohn-Sham (KS) equations. The generalized electronic exchange-correlation functional is described by generalized gradient approximation with the Perdew-Burke-Ernzerhof parametrization. The electron-ion interactions is described by pseudopotentials developed within the plane-wave basis projector augmented-wave (PAW) approach. These pseudopotentials are available at the VASP portal (http://cms.mpi.univie.ac.at/vasp/). Our calculations have been run with the pseudopotentials treating s and p semi-core states as valence in case for the elements Nb and Ti. The electronic densities and potentials are expanded over plane-waves with energy cutoff of 350 eV. 2x2x2 k-mesh and normal precision were used. The alloys were modeled by supercell containing 128 randomly distributed atoms. At initial step the atoms occupy perfect bcc lattice cites. This initial structure was optimized until energy changes less than 1e-6 eV, while forces acting on atoms don't exceed 1e-2 eV/angstrom. The electron-ion interaction is described by PAW pseudopotentials. The calculations have been collected by sampling chemical compositions across the entire compositional range. The chemical compositions have been sampled by progressively changing the number of atoms per constituent by 4. For each chemical composition of binaries and ternaries, the first-principle calculations have been run for 100 randomized arrangements of the constituents on the BCC lattice sites. We collected data for a total of 3,100 randomized atomic structures over 31 chemical compositions. The calculations have been collected on Air Force HPC11 cluster using the VASP 6.5.1. Additional methodology and file structure information is available in the dataset README.txt file.

36 MATERIALS SCIENCE↗
DOE OSTI2026

HfTi_BCC_SolidSolution_128atoms_VASP6

We performed density functional theory (DFT) calculations for body-centered-cubic (BCC) structures with 128 lattices sites of solid solution binary alloys hafnium-titanium (Hf-Ti). The electronic structures of alloys have been calculated using Vienna Ab initio Simulation Package (VASP). Within this package the DFT approach is used to reduce many-body Schrodinger equation to set of single particle Kohn-Sham (KS) equations. The generalized electronic exchange-correlation functional is described by generalized gradient approximation with the Perdew-Burke-Ernzerhof parametrization. The electron-ion interactions is described by pseudopotentials developed within the plane-wave basis projector augmented-wave (PAW) approach. These pseudopotentials are available at the VASP portal (http://cms.mpi.univie.ac.at/vasp/). Our calculations have been run with the pseudopotentials treating s and p semi-core states as valence in case for the elements Hf and Ti. The electronic densities and potentials are expanded over plane-waves with energy cutoff of 350 eV. 2x2x2 k-mesh and normal precision were used. The alloys were modeled by supercell containing 128 randomly distributed atoms. At initial step the atoms occupy perfect bcc lattice cites. This initial structure was optimized until energy changes less than 1e-6 eV, while forces acting on atoms don't exceed 1e-2 eV/angstrom. The electron-ion interaction is described by PAW pseudopotentials. The calculations have been collected by sampling chemical compositions across the entire compositional range. The chemical compositions have been sampled by progressively changing the number of atoms per constituent by 4. For each chemical composition of binaries and ternaries, the first-principle calculations have been run for 100 randomized arrangements of the constituents on the BCC lattice sites. We collected data for a total of 3,100 randomized atomic structures over 31 chemical compositions. The calculations have been collected on Air Force HPC11 cluster using the VASP 6.5.1. Additional methodology and file structure information is available in the dataset README.txt file.

36 MATERIALS SCIENCE↗
DOE OSTI2026

TiV_BCC_SolidSolution_128atoms_VASP6

We performed density functional theory (DFT) calculations for body-centered-cubic (BCC) structures with 128 lattices sites of solid solution binary alloys titanium-vanadium (Ti-V). The electronic structures of alloys have been calculated using Vienna Ab initio Simulation Package (VASP). Within this package the DFT approach is used to reduce many-body Schrodinger equation to set of single particle Kohn-Sham (KS) equations. The generalized electronic exchange-correlation functional is described by generalized gradient approximation with the Perdew-Burke-Ernzerhof parametrization. The electron-ion interactions is described by pseudopotentials developed within the plane-wave basis projector augmented-wave (PAW) approach. These pseudopotentials are available at the VASP portal (http://cms.mpi.univie.ac.at/vasp/). Our calculations have been run with the pseudopotentials treating s and p semi-core states as valence in case for the elements Ti and V. The electronic densities and potentials are expanded over plane-waves with energy cutoff of 350 eV. 2x2x2 k-mesh and normal precision were used. The alloys were modeled by supercell containing 128 randomly distributed atoms. At initial step the atoms occupy perfect bcc lattice cites. This initial structure was optimized until energy changes less than 1e-6 eV, while forces acting on atoms don't exceed 1e-2 eV/angstrom. The electron-ion interaction is described by PAW pseudopotentials. The calculations have been collected by sampling chemical compositions across the entire compositional range. The chemical compositions have been sampled by progressively changing the number of atoms per constituent by 4. For each chemical composition of binaries and ternaries, the first-principle calculations have been run for 100 randomized arrangements of the constituents on the BCC lattice sites. We collected data for a total of 3,100 randomized atomic structures over 31 chemical compositions. The calculations have been collected on Air Force HPC11 cluster using the VASP 6.5.1. Additional methodology and file structure information is available in the dataset README.txt file.

36 MATERIALS SCIENCE↗
DOE OSTI2025

HfTa_BCC_SolidSolution_128atoms_VASP6

We performed density functional theory (DFT) calculations for body-centered-cubic (BCC) structures with 128 lattices sites of solid solution binary alloys hafnium-tantalum (Hf-Ta). The electronic structures of alloys have been calculated using Vienna Ab initio Simulation Package (VASP). Within this package the DFT approach is used to reduce many-body Schrodinger equation to set of single particle Kohn-Sham (KS) equations. The generalized electronic exchange-correlation functional is described by generalized gradient approximation with the Perdew-Burke-Ernzerhof parametrization. The electron-ion interactions is described by pseudopotentials developed within the plane-wave basis projector augmented-wave (PAW) approach. These pseudopotentials are available at the VASP portal (http://cms.mpi.univie.ac.at/vasp/). Our calculations have been run with the pseudopotentials treating s and p semi-core states as valence in case for the elements Hf and Ta. The electronic densities and potentials are expanded over plane-waves with energy cutoff of 350 eV. 2x2x2 k-mesh and normal precision were used. The alloys were modeled by supercell containing 128 randomly distributed atoms. At initial step the atoms occupy perfect BCC lattice sites. This initial structure was optimized until energy changes less than 1e-6 eV, while forces acting on atoms don't exceed 1e-2 eV/angstrom. The electron-ion interaction is described by PAW pseudopotentials. The calculations have been collected by sampling chemical compositions across the entire compositional range. The chemical compositions have been sampled by progressively changing the number of atoms per constituent by 4. For each chemical composition of binaries and ternaries, the first-principle calculations have been run for 100 randomized arrangements of the constituents on the BCC lattice sites. We collected data for a total of 3,040 randomized atomic structures over 31 chemical compositions. Further methodological and structural information is contained in the dataset README.txt file.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Tight-Binding-Based Method for Simulations of Complex Materials with Accompanying Database

The NRL-Tight-Binding (NRL-TB) method has been applied successfully to many monatomic, binary, and a few ternary systems. The method consists of a fit to Density Functional Theory (DFT) results and has transferability beyond the fitted DFT database including performing tight-binding molecular dynamics simulations. We are working on a new website with a detailed guide of how to use the method in performing the fit to DFT results (Fitting Code) and obtaining non-orthogonal TB parameters expressed in a polynomial form as environment-dependent Slater-Koster parameters (on-site terms), and neighbor distance-dependent Hamiltonian and Overlap terms. These parameters are then used in a Static Code to verify or make predictions for large systems often beyond the computational capabilities of standard DFT codes. Our starting point was a website developed at NRL some years ago which NRL no longer supports. We have now been augmenting that website with new examples of expanding the original capabilities of the method such as incorporating in the codes f-electron states. Our website (esd.cos.gmu.edu/tb) contains two separate branches: One named NRL-TB with the full documentation of the method including source codes and examples. The other branch, named ESD-dB, is a library of electronic structure calculations for all the monatomic elements (a subset of the elements also found in a recent book by the author of this proposal. See reference 22) and an approximately 700 hundred compounds in specific crystal structures. We discuss below the progress made so far in improving and expanding the capabilities of our TB method and the plans for further extensions of our approach.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Machine Learned Force Field Modeling of Metal Organic Frameworks for CO2 Direct Air Capture

Direct air capture (DAC) is a method for removing CO2 directly from air. Metal organic frameworks (MOFs) have been studied as DAC sorbent materials because of their structural and chemical diversity. Thermodynamic calculations using classical force fields are often used to evaluate MOFs for their performance in separations such as CO2 capture. Machine-learned force fields (MLFFs) can use machine learning to form quantitative relationships between a material’s chemical structure and the forces and energies predicted by more accurate quantum mechanical calculations, such as dispersion-corrected density functional theory (DFT). These descriptions of forces and energies can be used to improve the accuracy of adsorption calculations. In this work, classical models were used to pre-screen MOFs for CO2 capture. DFT calculations were then used to examine the adsorption mechanism. Next, MLFF models were developed for MOFs to achieve DFT-level accuracy for the forces and energies associated with MOF flexibility and CO2 adsorption. These methods were parametrized based on thousands of DFT calculations of CO2 in flexible MOFs and used to predict MOF structural properties as well as CO2 adsorption properties.

Findley, John↗
DOE OSTI2024

Simple self-consistent method for excited states in density functional theory to characterize defect-derived behavior in wide-band-gap-based microelectronic materials

This final report summarizes the results of the Laboratory Direct Research and Development (LDRD) Project Number 229740. Wide band gap semiconductors such as gallium nitride (GaN) have features highly desirable for multiple mission electronic applications. Realization of their potential requires atomic-scale understanding of electronic behavior. The principal experimental tools for electronically probing defects in GaN are chemically undifferentiating and lack a practical theoretical counterpart needed to identify and characterize specific defects. This project investigated whether a simple idea for modeling defect excited states and their associated photoluminescence (PL) energies is viable, as a path to accelerate the understanding of defect behavior and gain valuable insights into engineering new electronic materials and devices. The research implemented a non-self-consistent total-energy evaluation of a Koopmans-type estimation of an excited electronic state energy in density functional theory (DFT) calculations, and proceeded to design, implement, and assess a self-consistent method for computing excited states based upon an OCcupation-Constrained-DFT (occ-DFT). The occ-DFT was verified in test calculations of defect excited states and validated against well-characterized PL data for 3d transition metal defects in GaN. The method proved stable and robust in computing excited states and gave accurate predictions compared to experimental PL data. The combined ground state/excited-state capability proved capable of chemically differentiating defect species in GaN. In application to 3d dopants in GaN, we reinterpreted extensive experimental literature, proposed new defects as prospective candidates for use in quantum information applications, and outlined design strategies to create and exploit these potentially useful functional defects in GaN.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Multi‐Scale Model‐Informed Deep Learning for Plasma‐Nanoparticle Interaction

The Overarching Goal of this proposed research is to understand and quantitively determine the interactions between non-thermal plasma (hot electrons, reactive radicals, vibrationally excited species) and surface reactions on influencing the activity and selectivity of the desired reactions via developing multi-scale model informed deep learning algorithm. Investigating non-thermal plasma-surface interaction is feasible due to the low bulk temperature in the discharge region. To investigate the role of plasma-nanoparticle interaction on enhancing the reaction kinetics, we will focus on ammonia cracking to generate clean hydrogen over earth-abundant, non-critical metallic nanoparticles, which is of great significance for decarbonization. We hypothesize that (1) reactive radicals interacting with surface reaction species via Eley–Rideal mechanism will significantly lower the energetics of the potential rate-limiting step of nitrogen formation; (2) the surface will be charged heterogeneously under non-thermal plasma conditions and the charged site will lower the energetics of ammonia cracking through Langmuir– Hinshelwood mechanism; (3) vibrationally excited ammonia will further promote the initial N-H bond cleavage. To access the hypothesis, we will (1) reveal the surface charge effects on tunning the reaction energetics via interpretable, physics-informed deep learning accelerated density functional theory (DFT) calculations; (2) determine the reactive radicals interacting with surface reaction species on tuning the reaction energetics via DFT; (3) reveal the surface charge effects on tunning the reaction energetics via DFT and deep learning models, (4) quantify how vibrationally excited species, reactive radicals, and surface charging effects on enhancing the catalysis via developing DFT-based microkinetic modeling (MKM) and active learning. Deep and active learning of plasma-nanoparticle interactions effects on enhancing ammonia cracking to generate hydrogen represents a new paradigm for designing high performance plasma materials. The fundamental science of how plasma-nanoparticle interactions will change the plasma kinetics and will improve the energy efficiency for decarbonization and sustainability. The interpretable and physics-informed machine learning model will accelerate low temperature plasma chemistry and material discovery with physics rules and model interpretation.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2023

Density functional modeling of the binding energies between aluminosilicate oligomers and different metal cations

Interactions between negatively charged aluminosilicate species and positively charged metal cations are critical to many important engineering processes and applications, including sustainable cements and aluminosilicate glasses. In an effort to probe these interactions, here we have calculated the pair-wise interaction energies (i.e., binding energies) between aluminosilicate dimer/trimer and 17 different metal cations M n+ (M n+ = Li + , Na + , K + , Cu + , Cu 2+ , Co 2+ , Zn 2+ , Ni 2+ , Mg 2+ , Ca 2+ , Ti 2+ , Fe 2+ , Fe 3+ , Co 3+ , Cr 3+ , Ti 4+ and Cr 6+ ) using a density functional theory (DFT) approach. Analysis of the DFT-optimized structural representations for the clusters (dimer/trimer + M n+ ) shows that their structural attributes (e.g., interatomic distances) are generally consistent with literature observations on aluminosilicate glasses. The DFT-derived binding energies are seen to vary considerably depending on the type of cations (i.e., charge and ionic radii) and aluminosilicate species (i.e., dimer or trimer). A survey of the literature reveals that the difference in the calculated binding energies between different M n+ can be used to explain many literature observations associated with the impact of metal cations on materials properties (e.g., glass corrosion, mineral dissolution, and ionic transport). Analysis of all the DFT-derived binding energies reveals that the correlation between these energy values and the ionic potential and field strength of the metal cations are well captured by 2nd order polynomial functions ( R 2 values of 0.99–1.00 are achieved for regressions). Given that the ionic potential and field strength of a given metal cation can be readily estimated using well-tabulated ionic radii available in the literature, these simple polynomial functions would enable rapid estimation of the binding energies of a much wider range of cations with the aluminosilicate dimer/trimer, providing guidance on the design and optimization of sustainable cements and aluminosilicate glasses and their associated applications. Finally, the limitations associated with using these simple model systems to model complex interactions are also discussed.

Gong, Kai↗
DOE OSTI2022

Machine learning prediction of the mechanical properties of refractory multicomponent alloys based on a dataset of phase and first principles simulation

In this work, a dataset including structural and mechanical properties of refractory multicomponent alloys was developed by fusing computations of phase diagram (CALPHAD) and density functional theory (DFT). The refractory multicomponent alloys, also named refractory complex concentrated alloys (CCAs) which contain 2–5 types of refractory elements were constructed based on Special Quasi-random Structure (SQS). The phase of alloys was predicted using CALPHAD and the mechanical property of alloys with stable and single body-centered cubic (BCC) at high temperature (over 1,500°C) was investigated using DFT-based simulation. As a result, a dataset with 393 refractory alloys and 12 features, including volume, melting temperature, density, energy, elastic constants, mechanical moduli, and hardness, were produced. To test the capability of the dataset on supporting machine learning (ML) study to investigate the property of CCAs, CALPHAD, and DFT calculations were compared with principal components analysis (PCA) technique and rule of mixture (ROM), respectively. It is demonstrated that the CALPHAD and DFT results are more in line with experimental observations for the alloy phase, structural and mechanical properties. Furthermore, the data were utilized to train a verity of ML models to predict the performance of certain CCAs with advanced mechanical properties, highlighting the usefulness of the dataset for ML technique on CCA property prediction.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Mechanical and Thermal Properties for Uranium and U–6Nb Alloy from First-Principles Theory

Elasticity, lattice dynamics, and thermal expansion for uranium and U–6Nb alloy (elastic moduli) are calculated from density functional theory that is extended to include orbital polarization (DFT+OP). Introducing 12.5 at.% of niobium, substitutionally, in uranium softens all the cii elastic moduli, resulting in a significantly softer shear modulus (G). Combined with a nearly invariant bulk modulus (B), the quotient B/G increases dramatically for U–6Nb, suggesting a more ductile material. Lattice dynamics from a harmonic model coupled with a DFT+OP electronic structure is applied for α uranium, and the obtained phonon density of states compares well with inelastic neutron-scattering measurements. The Debye temperature associated with the lattice dynamics falls within the range of experimentally observed Debye temperatures and it also validates our quasi-harmonic (QH) phonon model. The QH Debye–Grüneisen phonon method is combined with a DFT+OP electronic structure and used to explore the anisotropic thermal expansion in α uranium. The anomalous negative thermal expansion (contraction) of the b lattice parameter of the α-phase orthorhombic cell is relatively well reproduced from a free-energy model consisting of QH-phonon and DFT+OP electronic structure contributions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Electronic structure of compressively strained thin film La$_2$PrNi$_2$O$_7$

The discovery of superconductivity in the bulk nickelates under high pressure is a major advance in physics. The recent observation of superconductivity at ambient pressure in compressively strained bilayer nickelate thin films has now enabled direct characterization of the superconducting phase through angle resolved photoemission spectroscopy (ARPES). Here we present an in-situ ARPES study of compressively strained La$_2$PrNi$_2$O$_7$ films grown by oxide molecular beam epitaxy, and the ozone treated counterparts with an onset T$_c$ of 40 K, supplemented with results from pulsed laser deposition films with similar T$_c$. We resolve a systematic strain-driven electronic band shift with respect to that of bulk crystals, in qualitative agreement with density functional theory (DFT) calculations. However, the strongly renormalized flat 3$d_{z2}$ band shifts a factor of 5-10 smaller than anticipated by DFT. Furthermore, it stays ~70 meV below the Fermi level, contradicting the expectation that superconductivity results from the high density of states of this band at the Fermi level. We also observed a non-trivial k$_z$ dispersion of the cuprate-like 3$d_{x2-y2}$ band. Combined with results from both X-ray diffraction and DFT, we suggest that the strained films are under ~5 GPa effective pressure, considerably larger than the naïve expectation from the DFT relaxed structure. Finally, the ~70 meV energy position is intriguingly close to the collective mode coupling more prominently seen in thin films, in the energy range of both oxygen related phonons and the maximum of the spin excitation spectrum.

FOS: Physical sciences↗
DOE OSTI2025

2025 ASMS Investigation of the Collision-Induced Dissociation Mechanism of Protonated TODGA with IRIS

Title (20 words): Investigation of the Collision-Induced Dissociation Mechanism of Protonated TODGA with IRIS Introduction (120 words): One of the challenges facing wide-spread adoption of nuclear power is the development of efficient separation processes for used nuclear fuel. The molecules in separation processes are subjected to an extreme environment due to the high radiation fields from the used fuel and highly acidic media used for fuel dissolution, which results in significant molecular degradation, leading to reduced process efficiency. These degradation products must be identified and studied so mitigation strategies can be developed to maintain process efficiency. However, complex systems can have many degradation products, complicating identification. Untargeted analysis tools could be used to understand radiation chemistry in complex systems. However, this would necessitate improved understanding of the gas-phase fragmentation mechanisms of fuel cycle molecules like tetraoctyldiglycolamide (TODGA). Methods (120 words): The gas-phase fragmentation of protonated TODGA was investigated using collision-induced dissociation (CID), resonance ejection, and infrared ion spectroscopy (IRIS). CID and resonance ejection experiments were conducted using a Bruker Daltonics (Bremen, Gemany) SolariX XR fourier transform ion cyclotron resonance (FT-ICR) mass spectrometer. IRIS spectra of protonated TODGA and its two CID fragmentation products were measured using a modified Bruker amaZon Speed ETD 3D quadrupole ion trap mass spectrometer coupled to the Free Electron Lasers for Infrared eXperiments (FELIX) free electron laser. Measured spectra were compared with density functional theory (DFT) calculations using the Gaussian 16, Revision C.02 software package with the ?B97X-D functional and def2-TZVPP basis sets. Candidate structures were generated using the CREST 3.0 conformational sampling software tool. Preliminary Data (300 words): Collision-induced dissociation of protonated TODGA ([C36H73N2O3]+, m/z=581.562) results two fragment ions, one at m/z=340.285 assigned as [C20H38NO3]+ and the other at m/z=312.290, assigned as [C19H38NO2]+. Based on the assigned formula and the structure of protonated TODGA, the fragment at m/z=340.285 is likely formed from elimination of neutral dioctylamine. Comparison of the IRIS spectrum of m/z=340.285 with DFT predictions suggests it contains a ring structure, and is assigned as N-octyl-N-(6-oxo-1,4-dioxan-2-ylidene)octan-1-aminium. Based on this structure and the structure of protonated TODGA, we hypothesize this fragment formed from elimination of neutral dioctylamine followed by a ring closure mechanism. Comparison of the IRIS spectrum of the fragment at m/z=312.290 with DFT predictions also indicated the presence of a ring structure, assigned as N-(1,3-dioxolan-4-ylidene)-N-octyloctan-1-aminium. This product could be formed from elimination of carbon monoxide from the ring of m/z=340.285 as a sequential fragmentation or formed directly from protonated TODGA via elimination of neutral N,N-dioctylformamide followed by a ring closure. Resonance ejection experiments where m/z=340 was continuously ejected from the IRC cell showed no decrease in intensity of m/z=312.290 across several collision energies, suggesting that the later, direct formation mechanism, dominates. The location of the ionizing proton in protonated TODGA is important for modeling the fragmentation mechanisms. DFT calculations suggested that the position of bands involving the coupled vibrations of the amide C—N and C=O bonds in TODGA are the most sensitive to proton location. Evaluation of the IRIS spectrum of protonated TODGA suggests that the ionizing proton is located between the two amid oxygens. This protonation location was calculated to lie approximately 30 kJ/mol lower in energy than the next lowest energy location, with the proton located solely on one of the amide oxygens. Novel aspect (20 words): Infrared ion spectroscopy combined with resonance ejection experiments and density functional theory to probe the collision-induced dissociation mechanism of tetraoctyldiglycolamide.

37 - INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL C↗
DOE OSTI2025

Static Subspace Approximation for Random Phase Approximation Correlation Energies: Applications to Materials for Catalysis and Electrochemistry

Modeling complex materials using high-fidelity, ab initio methods at low cost is a fundamental goal for quantum chemical software packages. The GW approximation and random phase approximation (RPA) provide a unified description of both electronic structure and total energies using the same physics in a many-body perturbative approach that can be more accurate than generalized-gradient density functional theory (DFT) methods. However, GW/RPA implementations have historically been limited to either specific materials classes or application toward small chemical systems. Here, the static subspace approximation allows for reduced cost full-frequency GW/RPA calculations and has previously been benchmarked thoroughly for GW calculations. Here, we describe our approach to including partial occupations of electronic orbitals in full-frequency GW and RPA calculations for the study of electrocatalysts. We benchmarked RPA total energy calculations using the subspace approximation across a diverse test suite of materials for a variety of computational parameters. The benchmarking quantifies the impact of different extrapolation procedures for representing the static polarizability at infinite screened cutoff, and shows that using screened cutoffs above 20-25 Ryd result in diminishing accuracy returns for predicting RPA total energies. Additionally, for moderately sized electrocatalytic models, 2-3 times fewer computational resources are used to compute RPA total energies by representing the static polarizability with 20-30% of the static subspace basis, with an error of approximately 0.01 eV or better in RPA adsorption energy calculations. Finally, we show that for these electrochemical models RPA can shift DFT adsorption energy shifts by up to 0.5 eV and that GW can frequently shift DFT eigenvalues of surface and adsorbate states by approximately 0.5-1 eV.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Data on the comprehensive first-principles diffusion study of the aluminum-magnesium system

First-principles calculation of diffusion coefficients between Mg and Al is investigated comprehensively using density functional theory (DFT). The effect of different uncertainty sources arising from first principles calculations has been investigated systematically. These sources include the diffusion model, energetic, entropic and attempt frequency calculations. Variation in self and impurity diffusion coefficients of Mg and Al in stable phases are quantified using different DFT settings and compared with the experiments. Using the optimal DFT settings, diffusion coefficients in metastable phases of Al and Mg are predicted. The dataset refers to “An integrated experimental and computational study of diffusion and atomic mobility of the aluminum-magnesium system” [1].

36 MATERIALS SCIENCE↗
DOE OSTI2021

First-principles investigation of uranium mononitride (UN): Effect of magnetic ordering, spin-orbit interactions and exchange correlation functional

Uranium mononitride (UN) is a promising nuclear fuel that combines the advantageous properties of readily used UO 2 and uranium alloys. Various properties of UN have been previously studied using different density functional theory (DFT) methodologies; however, there are still inconsistencies when it comes to the dynamical stability and defect properties of UN. We address these inconsistencies by studying the UN phonons and defect properties using DFT calculations employing two generalized gradient approximation (GGA) exchange-correlation functionals: PBE and AM05, with and without an added on-site Coulomb repulsion term (+U). Furthermore, we investigate the importance of spin-orbit coupling (SOC) when calculating the properties of UN. We use the different methodologies to determine the preference of UN to have antiferromagnetic (AFM) ordering, as seen in experiments, or ferromagnetic (FM) ordering of the uranium spins. We compare the crystallographic properties, density of states, the DFT X-ray photoelectron spectra and phonon dispersions calculated using the different methodologies. We demonstrate that GGA + U reproduces the AFM ordering in UN, but the crystal structure is dynamically unstable. We also show that magnetic ordering is important in finding the lowest energy defective structure, and that SOC has a distinct influence on the energy of the different uranium interstitial defects. Lastly, we discuss the point defect formation energies under U-rich and N-rich conditions, and the stoichiometric formation energies calculated with the different methodologies, providing insight into the observed tendency for forming hypostoichiometric UN.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Multiscale study of helium diffusion in Ni-Cr alloys: Short-range trapping versus long-range channeling

Ni-Cr alloys are widely employed as structural materials in fast nuclear reactors but are vulnerable to high-temperature helium (He) embrittlement (HTHE) under fast neutron irradiation. A comprehensive understanding of He diffusion in Ni-Cr alloys, which governs the kinetics of HTHE, is therefore essential for developing resilient materials and preventing failure. In this work, we reveal the underlying mechanisms of He diffusion in pure Ni and Ni-Cr alloys by integrating density functional theory (DFT) with atomic kinetic Monte Carlo (AKMC) simulations. Our findings uncover a non-monotonic dependence of He diffusivity on Cr concentration, contradicting the monotonic trends predicted by DFT-parameterized theories. At low Cr concentrations, He diffusion is dominated by short-range trapping, characterized by multiple trapping sites and a distinct mechanism within the first nearest neighbor of Cr, differing from that in pure Ni. At high Cr concentrations, these local traps become interconnected, forming long-range fast diffusion channels that enhance He mobility. The competition between localized trapping and extended channeling results in a diffusivity that first decreases, then increases with rising Cr content. These atomic-scale insights offer critical guidance for the design of radiation-tolerant Ni-based alloys. Moreover, the combined DFT-AKMC methodology and the concept of random walker diffusion through interconnected energy basins present a broadly applicable framework for studying transport phenomena in disordered systems.

36 - MATERIALS SCIENCE↗
DOE OSTI2021

Stability and mobility of tungsten clusters on tungsten (110) surface: Ab initio and atomistic simulations

Quantifying the surface transport properties of tungsten (W) is of prime importance to understand the formation of nano-fuzz in fusion plasma-facing conditions. The stability and mobility of W adatom clusters (W n , n = 2-9) on the W(110) surface has been investigated by computer simulations, including ab initio calculations using density functional theory (DFT) and molecular statics (MS) simulations with multiple W interatomic potentials. The DFT results demonstrate that the sequential binding energy generally increases with number of W adatoms, except for the 5 th and 7 th W adatoms. The most common elemental migration steps of W n (n>2) clusters are observed to consist of monomer and dimer hops, while larger W n clusters can also diffuse by dissociation and recombination of smaller clusters. The threshold migration energy of W 9 is the highest, then followed by W 8 , W 4 , and W 6 , while W 3 , W 5 , and W 7 have similar migration energies. Compared to DFT, each interatomic potential evaluated overestimates the binding energies of W n clusters. Additionally, the embedded-atom potential developed by Juslin and Wirth adequately predicts the threshold migration energy of W n (n>2) clusters, although it predicts different underlying migration mechanisms. The results show that interaction mechanism between W adatoms controls the stability and mobility of W n clusters on the W(110) surface.

36 MATERIALS SCIENCE↗