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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 OSTI2021

H-Atom Assignment and Sb–O Bonding of [Mes 3 SbOH][O 3 SPh] Confirmed by Neutron Diffraction, Multipole Modeling, and Hirshfeld Atom Refinement

Neutron wavelength-resolved Laue diffraction experiments permit accurate refinement of the H-atom positions and anisotropic displacement parameters of [Mes 3 SbOH][O 3 SPh]. A multipole-based charge density refinement and a topological analysis of the refined electron density were also performed. Hirshfeld atom refinement (HAR) recovers the neutron-determined H-atom parameters, and the quantum-mechanical electron density used in HAR recovers the electron density topology from the refined multipole model. We report these results confirm that [Mes 3 SbOH][O 3 SPh] does indeed feature a hydroxystibonium cation with a nominal Sb–O single bond and not a stibine oxide with an Sb=O/Sb + –O – bond.

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

Capturing Correlation Effects in Positron Binding to Atoms and Molecules

A major challenge in contemporary electronic structure theory involves the development of methods to describe in a balanced manner the contribution of correlation effects to energy differences. This challenge can be even greater for multicomponent systems containing more than one type of quantum particle. In the present work, we describe a flexible code for carrying out self-consistent field and configuration interaction (CI) calculations on multicomponent systems and use it to generate trial wave functions for use in diffusion Monte Carlo (DMC) calculations of the positron affinity of Be, Be 2 , Be 4 , Mg, CS 2 , and benzene. The resulting positron affinities (PAs) are in good agreement with the best values from the literature.

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

Intersystem crossing and exciton–defect coupling of spin defects in hexagonal boron nitride

Despite the recognition of two-dimensional (2D) systems as emerging and scalable host materials of single-photon emitters or spin qubits, the uncontrolled, and undetermined chemical nature of these quantum defects has been a roadblock to further development. Leveraging the design of extrinsic defects can circumvent these persistent issues and provide an ultimate solution. Here, we established a complete theoretical framework to accurately and systematically design quantum defects in wide-bandgap 2D systems. With this approach, essential static and dynamical properties are equally considered for spin qubit discovery. In particular, many-body interactions such as defect–exciton couplings are vital for describing excited state properties of defects in ultrathin 2D systems. Meanwhile, nonradiative processes such as phonon-assisted decay and intersystem crossing rates require careful evaluation, which competes together with radiative processes. From a thorough screening of defects based on first-principles calculations, we identify promising single-photon emitters such as Si VV and spin qubits such as Ti VV and Mo VV in hexagonal boron nitride. This work provided a complete first-principles theoretical framework for defect design in 2D materials.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Iron telluride ladder compounds: Predicting the structural and magnetic properties of BaFe 2 Te 3

Since the discovery of pressure-induced superconductivity in the two-leg ladder system BaFe 2 X 3 (X=S, Se), with the 3d iron electronic density n=6, quasi-one-dimensional iron-based ladders have attracted considerable attention. In this work, we use density-functional theory to predict that the novel n=6 iron ladder BaFe 2 Se 3 could be stable with a similar crystal structure as BaFe 2 Se 3 . Furthermore, our results also indicate that BaFe2Te3 will display a complex 2×2 block-type magnetic order. Due to the magnetic striction effects of this block order, BaFe2Te3 should be a magnetic noncollinear ferrielectric system with a net polarization 0.31μC/cm2. In summary, the similar electronic density and magnetic ground state of Te- and Se-based ladders indicates both should display similar properties. In particular, the physical and structural similarity with BaFe 2 Se 3 suggests that BaFe 2 Se 3 could become superconducting under high pressure.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Dynamic mode decomposition for extrapolating nonequilibrium Green's-function dynamics

The Hartree-Fock generalized Kadanoff-Baym ansatz (HF-GKBA) offers an approximate numerical procedure for propagating the two-time nonequilibrium Green's function (NEGF). Here, using the GW self-energy, we compare the HF-GKBA to exact results for a variety of systems with long- and short-range interactions, different two-body interaction strengths, and various nonequilibrium preparations. We find excellent agreement between the HF-GKBA and exact time evolution in models when more realistic long-range exponentially decaying interactions are considered. Furthermore, this agreement persists for long times and for intermediate to strong interaction strengths. In large systems, HF-GKBA becomes prohibitively expensive for long-time evolutions. For this reason, we look at the use of dynamical mode decomposition (DMD) to reconstruct long-time NEGF trajectories from a sample of the initial trajectory. Using no more than 16% of the total time evolution, we reconstruct the total trajectory with high fidelity. Our results show the potential for DMD to be used in conjunction with HF-GKBA to calculate long-time trajectories in large-scale systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Imposing correct jellium response is key to predict the density response by orbital-free DFT

Orbital-free density functional theory constitutes a computationally highly effective tool for modeling electronic structures of systems ranging from room-temperature materials to warm dense matter. Its accuracy critically depends on the employed kinetic energy (KE) density functional, which has to be supplied as an external input. In this work we consider several nonlocal and Laplacian-level KE functionals and use an external harmonic perturbation to compute the static density response at T = 0 K in the linear and beyond-linear response regimes. We test for the satisfaction of exact conditions in the limit of uniform densities and for how approximate KE functionals reproduce the density response of realistic materials (e.g., Al and Si) against the Kohn-Sham DFT reference, which employs the exact KE. The results illustrate that several functionals violate exact conditions in the uniform electron gas (UEG) limit. We find a strong correlation between the accuracy of the KE functionals in the UEG limit and in the strongly inhomogeneous case. This empirically demonstrates the importance of imposing the limit of UEG response for uniform densities and validates the use of the Lindhard function in the formulation of kernels for nonlocal functionals. This conclusion is substantiated by additional calculations for bulk aluminum (Al) with a face-centered cubic (fcc) lattice and silicon (Si) with an fcc lattice, body-centered cubic (bcc) lattice, and semiconducting crystal diamond state. The analysis of fcc Al, and fcc as well as bcc Si data follows closely the conclusions drawn for the UEG, allowing us to extend our conclusions to realistic systems that are subject to density inhomogeneities induced by ions.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

GraphEM

An unsupervised segmentation method for structural analysis of Scanning Transmission Electron Microscopy (STEM) images

Pope, Jenna↗
DOE OSTI2024

VitroJet: new features and case studies

Single-particle cryo-electron microscopy has become a widely adopted method in structural biology due to many recent technological advances in microscopes, detectors and image processing. Before being able to inspect a biological sample in an electron microscope, it needs to be deposited in a thin layer on a grid and rapidly frozen. The VitroJet was designed with this aim, as well as avoiding the delicate manual handling and transfer steps that occur during the conventional grid-preparation process. Since its creation, numerous technical developments have resulted in a device that is now widely utilized in multiple laboratories worldwide. It features plasma treatment, low-volume sample deposition through pin printing, optical ice-thickness measurement and cryofixation of pre-clipped Autogrids through jet vitrification. This paper presents recent technical improvements to the VitroJet and the benefits that it brings to the cryo-EM workflow. A wide variety of applications are shown: membrane proteins, nucleosomes, fatty-acid synthase, Tobacco mosaic virus, lipid nanoparticles, tick-borne encephalitis viruses and bacteriophages. These case studies illustrate the advancement of the VitroJet into an instrument that enables accurate control and reproducibility, demonstrating its suitability for time-efficient cryo-EM structure determination.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

The importance of correlation in the molecular orbital picture

The molecular orbital picture plays a fundamental role in analyzing and interpreting the electronic structure of atoms and molecules. Evaluation of molecular orbitals obtained from the Hartree–Fock method and other one-electron Hamiltonian models is routine for quantum-chemical studies. Although these analyses have proven to be useful for identifying different patterns in electronic structure and reactivity, in many cases, the chosen set of orbitals do not incorporate many of the fundamental electron correlation effects needed to accurately describe the atom or molecule under study. This work addresses the question of whether or not the inclusion of electron correlation is essential for the orbital picture by contrasting the differences between canonical Hartree–Fock orbitals and the correlated, normalized Dyson orbitals.

Hernandez Corzo, Hector↗
DOE OSTI2020

Ab Initio Study of Stability, Local Order, and Phase Diagram For a Series of bcc-based Transition Metal Alloys

In this work, a parameter-free electronic structure approach is applied to the study of stability and chemical order in the 15 substitutional body-centered cubic (bcc)-based alloys made of the six transition metals of groups 5 (V, Nb, Ta) and 6 (Cr, Mo, W) of the periodic table. The method is based on a Green’s function description of the electronic structure of the random alloys. Configurational order is treated within the generalized perturbation method, and temperature effects are examined with a generalized mean-field approach. In contrast to the results summarized in the assessed phase diagrams, stability and ordering trends are predicted in a broad range of alloy composition for at least seven alloys, and explanation is found in their electronic structure properties. Short-range order results, thermodynamics analysis, and bcc-based phase diagrams are also presented.

36 MATERIALS SCIENCE↗
DOE OSTI2021

PyCCE: A python package for custer correlation expansion simulations of spin qubit dynamics.

PyCCE, an open-source Python library for simulating the dynamics of spin qubits in a spin bath, is presented using the cluster-correlation expansion (CCE) method. PyCCE includes modules to generate realistic spin baths, employing coupling parameters computed from first principles with electronic structure codes, and enables the user to run simulations with either the conventional or generalized CCE method. Three use cases of the Python library are illustrated: the calculation of the Hahn-echo coherence time of the nitrogen-vacancy in diamond; the calculation of the coherence time of the basal divacancy in silicon carbide at avoided crossings; and the calculation for magnetic field orientation-dependent dynamics of a shallow donor in silicon. The complete documentation, downloadable tutorials, and installation instructions are available at https://pycce.readthedocs.io/en/latest/.

coherence↗
DOE OSTI2020

P SI4 1.4: Open-source software for high-throughput quantum chemistry

PSI4 is a free and open-source ab initio electronic structure program providing implementations of Hartree–Fock, density functional theory, many-body perturbation theory, configuration interaction, density cumulant theory, symmetry-adapted perturbation theory, and coupled-cluster theory. Most of the methods are quite efficient, thanks to density fitting and multi-core parallelism. The program is a hybrid of C++ and Python, and calculations may be run with very simple text files or using the Python API, facilitating post-processing and complex workflows; method developers also have access to most of PSI4 's core functionalities via Python. Job specification may be passed using The Molecular Sciences Software Institute (MolSSI) QCSCHEMA data format, facilitating interoperability. We announce a rewrite of our top-level computation driver, and concomitant adoption of the MolSSI QCARCHIVE INFRASTRUCTURE project, makes the latest version of PSI4 well suited to distributed computation of large numbers of independent tasks. The project has fostered the development of independent software components that may be reused in other quantum chemistry programs.

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

Intercalation as a versatile tool for fabrication, property tuning, and phase transitions in 2D materials

Recent advances in two-dimensional (2D) materials have led to the renewed interest in intercalation as a powerful fabrication and processing tool. Intercalation is an effective method of modifying the interlayer interactions, doping 2D materials, modifying their electronic structure or even converting them into starkly different new structures or phases. Herein, we discuss different methods of intercalation and provide a comprehensive review of various roles and applications of intercalation in next-generation energy storage, optoelectronics, thermoelectrics, catalysis, etc. The recent progress in intercalation effects on crystal structure and structural phase transitions, including the emergence of quantum phases are also reviewed.

2D materials↗
DOE OSTI2022

Physical properties and electronic structure of single-crystal KCo 2 As 2

We present a method for producing high quality KCo 2 As 2 crystals, stable in air and suitable for a variety of measurements. X-ray diffraction, magnetic susceptibility, electrical transport and heat capacity measurements confirm the high quality and an absence of long range magnetic order down to at least 2 K. Residual resistivity values approaching 0.25 µΩ cm are representative of the high quality and low impurity scattering, and a Sommerfeld coefficient γ = 7.3 mJ/mol K 2 signifies weaker correlations than the Fe-based counterparts. Together with Hall effect measurements, angle-resolved photoemission experiments reveal a Fermi surface consisting of electron pockets at the center and corner of the Brillouin zone, in line with theoretical predictions and in contrast to the mixed carrier types of other pnictides with the ThCr 2 Si 2 structure. A large, linear magnetoresistance of 200% at 14 T, together with an observed linear and hyperbolic, rather than parabolic, band dispersions are unusual characteristics of this compound.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

A Particle Method for the Multispecies Landau Equation

Abstract The multispecies Landau collision operator describes the two-particle, small scattering angle or grazing collisions in a plasma made up of different species of particles such as electrons and ions. Recently, a structure preserving deterministic particle method (Carrillo et al. in J. Comput. Phys. 7:100066, 2020) has been developed for the single species spatially homogeneous Landau equation. This method relies on a regularization of the Landau collision operator so that an approximate solution, which is a linear combination of Dirac delta distributions, is well-defined. Based on a weak form of the regularized Landau equation, the time dependent locations of the Dirac delta functions satisfy a system of ordinary differential equations. In this work, we extend this particle method to the multispecies case, and examine its conservation of mass, momentum, and energy, and decay of entropy properties. We show that the equilibrium distribution of the regularized multispecies Landau equation is a Maxwellian distribution, and state a critical condition on the regularization parameters that guarantees a species independent equilibrium temperature. A convergence study comparing an exact multispecies Bobylev-Krook-Wu (BKW) solution to the particle solution shows approximately 2nd order accuracy. Important physical properties such as conservation, decay of entropy, and equilibrium distribution of the particle method are demonstrated with several numerical examples.

Mathematics↗
DOE OSTI2022

Single- and two-particle finite size effects in interacting lattice systems

Simulations of extended quantum systems are typically performed by extrapolating results of a sequence of finite-system-size simulations to the thermodynamic limit. In the quantum Monte Carlo community, twist-averaging was pioneered as an efficient strategy to eliminate one-body finite size effects. In the dynamical mean field community, cluster generalizations of the dynamical mean field theory were formulated to study systems with nonlocal correlations. In this work, we put the twist-averaging and the dynamical cluster approximation variant of the dynamical mean field theory onto equal footing, discuss commonalities and differences, and compare results from both techniques to the standard periodic boundary technique. At the example of Hubbard-type models with local, short-range and Yukawa-like longer range interactions we show that all methods converge to the same limit, but that the convergence speed differs in practice. We show that embedding theories are an effective tool for managing both one-body and two-body finite size effects, in particular if interactions are averaged over twist angles.

36 MATERIALS SCIENCE↗