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Results for “projector augmented wave method”

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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59 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

A Filon-like integration strategy for calculating exact exchange in periodic boundary conditions: a plane-wave DFT implementation

An efficient and accurate approach for calculating exact exchange and other two-electron integrals has been developed for periodic electronic structure methods. Traditional approaches used for integrating over the Brillouin zone in band structure calculations, e.g. trapezoidal or Monkhorst-Pack, are not accurate enough for two-electron integrals. This is because their integrands contain multiple singularities over the double integration of the Brillouin zone, which with simple integration methods lead to very inaccurate results. A common approach to this problem has been to replace the Coulomb interaction with a screened Coulomb interaction that removes singularities from the integrands in the two-electron integrals, albeit at the inelegance of having to introduce a screening factor which must precomputed or guessed. Instead of introducing screened Coulomb interactions in an ad hoc way, the method developed in this work derives an effective screened potential using a Filon-like integration approach that is based only on the lattice parameters. This approach overcomes the limitations of traditionally defined screened Coulomb interactions for calculating two-electron integrals, and makes chemistry many-body calculations tractable in periodic boundary conditions. This method has been applied to several systems for which conventional DFT methods do not work well, including the reaction pathways for the addition of H 2 to phenol and Au$^{–}_{20}$ nanoparticle, and the electron transfer of a charge trapped state in the Fe(II) containing mica, annite.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Accelerating Embedding Potential Optimization by Reconstructing the Pseudo-Valence Electron Density

Density functional embedding theory (DFET) enables use of electronic structure methods with higher accuracy than density functional theory in a local region, with applications thus far ranging from (photo/electro)catalysis to reactions in solution. DFET partitions a large collection of atoms into smaller groups that interact via a shared embedding (interaction) potential V emb , determined via functional optimization. The optimized effective potential (OEP) process used to optimize V emb is time-consuming and becomes a computational bottleneck due to sharp, oscillating features of V emb near nuclei. Here, similar to pseudopotential theory, by reconstructing electron densities used in the OEP process from smoother pseudo-valence-only (PVO) electron densities as proxies for total densities of the full system and subsystems, we can retain accuracy in the embedded electronic structure calculations while potentially reducing the overhead of V emb construction, within the projector augmented-wave (PAW) formalism. We explore three different chemical reactions as exemplars to test PVO–DFET, namely, H 2 dissociative adsorption on a Cu(111) surface, H 2 O adsorption on a Pt(111) surface, and aqueous [Ca 2+ –SO 4 2– ] ion-pair formation. The PVO approximation works well for all three systems with minimal loss of accuracy (∼10–70 meV error relative to the original exact-derivative (ED) approach) while accelerating V emb generation for the Cu and Pt systems respectively by 20× and 5×. Given proper numerical convergence parameters, the spatial distributions of differences between PVO- and ED-based V emb outside the core regions are small, explaining the exceptional agreement between the two approaches. Finally, we anticipate that this more efficient PVO–DFET approximation will be useful whenever computation of V emb is much more expensive than subsequent embedded high-level electron correlation calculations.

approximation↗
DOE OSTI2012

First-principles calculations of the stability and incorporation of helium, xenon and krypton in uranium

While metallic fuels have a long history of reactor use, their fundamental physical and thermodynamic properties are not well understood. Many metallic nuclear fuels are body-centered cubic alloys of uranium that swell under fission conditions, creating fission product gases such as helium, xenon and krypton. In this paper, helium, xenon, and krypton point defects are investigated in the a and ? phases of metallic uranium using first principles calculations. A density functional theory (DFT) framework is utilized with projector augmented-wave (PAW) pseudopotentials. Formation and incorporation energies of He, Xe, and Kr are calculated at various defect positions for the prediction of fission gas behavior in uranium. In most cases, defect energies follow a size effect, with helium incorporation and formation energies being the smallest. The most likely position for the larger Xe and Kr atoms in uranium is the substitutional site. Helium atoms are likely to be found in a wide variety of defect positions due to the comparable formation energies of all defect configurations analyzed. This is the first detailed study of the stability and incorporation of fission gases in uranium.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2011

Simple concentration-dependent pair interaction model for large-scale simulations of Fe-Cr alloys

This work is motivated by the need for large-scale simulations to extract physical information on the iron-chromium system that is a binary model alloy for ferritic steels used or proposed in many nuclear applications. From first-principles calculations and the experimental critical temperature we build a new energetic rigid lattice model based on pair interactions with concentration and temperature dependence. Density functional theory calculations in both norm-conserving and projector augmented-wave approaches have been performed. A thorough comparison of these two different ab initio techniques leads to a robust parametrization of the Fe-Cr Hamiltonian. Mean-field approximations and Monte Carlo calculations are then used to account for temperature effects. The predictions of the model are in agreement with the most recent phase diagram at all temperatures and compositions. The solubility of Cr in Fe below 700 K remains in the range of about 6 to 12%. It reproduces the transition between the ordering and demixing tendency and the spinodal decomposition limits are also in agreement with the values given in the literature.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Absorption and diffusion of oxygen in the Ti{sub 3}Al alloy

The absorption and diffusion of oxygen in the Ti{sub 3}Al alloy are studied by the projector augmented wave within the density functional theory. The highest absorption energies are shown to correspond to the sites in the octahedra formed by six titanium atoms, and the presence of aluminum in the nearest neighbors leads to a substantial decrease in the binding energy of oxygen in the alloy by approximately 1.5 eV. The energy barriers of oxygen diffusion between various interstices in the crystal lattice of the alloy are estimated, and the preferred migration paths in the (0001) plane and the [0001] direction are determined. It is found that the migration barrier from the most preferred octahedral O1 site to distorted tetrahedral Ti-site (2.42 eV) is a key barrier and limits the oxygen diffusion in the alloy. The calculated temperature diffusion coefficient of oxygen in the Ti{sub 3}Al alloy and the activation energies determined in two directions agree with the experimental data.

36 MATERIALS SCIENCE↗