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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 631 records · Page 35
All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

Structure Analysis of a Precipitate Phase in an Ni-Rich High Temperature NiTiHf Shape Memory Alloy

Thermal aging of the high temperature shape memory alloy 50.3Ni-29.7Ti-20Hf (at.%) introduces a novel precipitate phase, which plays an important role in improving shape memory properties. The precipitate phase was investigated by conventional electron diffraction, high resolution scanning transmission electron microscopy (STEM) and three dimensional atom probe tomography. An unrelaxed orthorhombic atomic structural model is proposed based on these observations. This model was subsequently relaxed by ab initio calculations. As a result of the relaxation, atom shuffle displacements occur, which in turn yields improved agreement with the STEM images. The relaxed structure, which is termed the “H-phase”, has also been verified to be thermodymanically stable at 0 K.

Atom probe tomography, Ni-Ti-Hf alloy, shape memor↗
DOE OSTI2022

Data-centric framework for crystal structure identification in atomistic simulations using machine learning

Atomic-level modeling performed at large scales enables the investigation of mesoscale materials properties with atom-by-atom resolution. The spatial complexity of such cross-scale simulations renders them unsuitable for simple human visual inspection. Instead, specialized structure characterization techniques are required to aid interpretation. These have historically been challenging to construct, requiring significant intuition and effort. Here we propose an alternative framework for a fundamental structural characterization task: classifying atoms according to the crystal structure to which they belong. Our approach is data-centric and favors the employment of Machine Learning over heuristic rules of classification. A group of data-science tools and simple local descriptors of atomic structure are employed together with an efficient synthetic training set. We also introduce the first standard and publicly available benchmark data set for evaluation of algorithms for crystal-structure classification. Further, it is demonstrated that our data-centric framework outperforms all of the most popular heuristic methods—especially at high temperatures when lattices are the most distorted—while introducing a systematic route for generalization to new crystal structures. Moreover, through the use of outlier detection algorithms our approach is capable of discerning between amorphous atomic motifs (i.e., noncrystalline phases) and unknown crystal structures, making it uniquely suited for exploratory materials synthesis simulations.

36 MATERIALS SCIENCE↗
NASA NTRS1985

Theoretical quasar emission-line ratios. VII - Energy-balance models for finite hydrogen slabs

The present energy balance calculations for finite, isobaric, hydrogen-slab quasar emission line clouds incorporate probabilistic radiative transfer (RT) in all lines and bound-free continua of a five-level continuum model hydrogen atom. Attention is given to the line ratios, line formation regions, level populations and model applicability results obtained. H lines and a variety of other considerations suggest the possibility of emission line cloud densities in excess of 10 to the 10th/cu cm. Lyman-beta/Lyman-alpha line ratios that are in agreement with observed values are obtained by the models. The observed Lyman/Balmer ratios can be achieved with clouds whose column depths are about 10 to the 22nd/sq cm.

Hubbard, E. N.↗
NASA NTRS1988

A partially collisional model of the Titan hydrogen torus

Occasional collision effects are encompassed by the present numerical model of atomic hydrogen densities in Titan's hydrogen torus, which is noted to be azimuthally symmetric; the torus density peaks sharply at Titan's orbit, and rapidly decreases in the both radially outward and perpendicular directions. Collisions of Saturnian atoms with the torus population produce a corona. Without this coronal population, the torus model would not reproduce the Voyager 2 Lyman-alpha intensities. These observations may nevertheless be modelled by a torus-plus-corona model that also reconciles the Pioneer 11 torus observations with those of the two Voyager spacecraft.

Hilton, Douglas A.↗
DOE OSTI2017

Detailed, sterically-resolved modeling of soot oxidation: Role of O atoms, interplay with particle nanostructure, and emergence of inner particle burning

A newly-developed detailed mechanism of soot oxidation was tested against experimental observations. The computations were performed at an atomistic level and with a detailed consideration of soot particle surface sites. Several additional reactions were investigated theoretically and one of them, oxidation of embedded five-member rings by O atoms, was included in the model. Here, the primary focus of the study was on the high-temperature shock-tube experiments of Roth et al. (1991). The reaction model was able to reproduce the experimental results, but required coupling to particle nanostructure: partial oxidation of PAH molecules and the decrease in PAH initial sizes along the oxidation path. The principle reaction mechanism was identified to be the formation of oxyradicals, their decomposition, formation of hard-to-oxidize embedded five-member rings, and oxidation of the latter predominantly by O atoms. The analysis identified O as the most effective oxidizer of the embedded five-member rings, which thus controls the rate of the overall oxidation. The model thus predicts fast oxidation during a brief initial period followed by a slow-oxidation one. The model of partial oxidation of an aromatic molecule and switching to the next intact molecule suggests pore formation and subsequent inner particle burning. We also investigated the ability of the present model to reproduce recent measurements of soot oxidation rates performed by Camacho et al. (2015) at about 1000 K. The initial reaction model failed to predict these results, and no adjustment could reconcile the differences. The only way to bring the model to experimental values was by assuming a catalytic decomposition of water on the reactor wall supplying additional radicals, H and OH, to the reacting gas mixture. Additional chemistry, oxidation through complex formation at neighboring surface sites, was required to fully reproduce the experimental observations. These additional reactions were found to play no role in the high-temperature simulations, nor were they sufficient to reproduce the low-temperature experiment on their own, without the assumed catalytic decomposition of water.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Decomposition of the configuration-interaction coefficients in the multiconfiguration time-dependent Hartree-Fock method

An approximate implementation of the multiconfiguration time-dependent Hartree-Fock method is proposed, in which the matrix of configuration-interaction coefficients is decomposed into a product of matrices of smaller dimension. The applicability of this method in which all the configurations are kept in the expansion of the wave function, while the configuration-interaction coefficients are approximately calculated, is discussed by showing the results on three model systems: a one-dimensional model of a beryllium atom, a one-dimensional model of a carbon atom, and a one-dimensional model of a chain of four hydrogen atoms. The time-dependent electronic dynamics induced by a few-cycle, long-wavelength laser pulse is found to be well described at a lower computational cost compared to the standard multiconfiguration time-dependent Hartree-Fock treatment. Drawbacks of the method are also discussed.

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

TEMImageNet training library and AtomSegNet deep-learning models for high-precision atom segmentation, localization, denoising, and deblurring of atomic-resolution images

Abstract Atom segmentation and localization, noise reduction and deblurring of atomic-resolution scanning transmission electron microscopy (STEM) images with high precision and robustness is a challenging task. Although several conventional algorithms, such has thresholding, edge detection and clustering, can achieve reasonable performance in some predefined sceneries, they tend to fail when interferences from the background are strong and unpredictable. Particularly, for atomic-resolution STEM images, so far there is no well-established algorithm that is robust enough to segment or detect all atomic columns when there is large thickness variation in a recorded image. Herein, we report the development of a training library and a deep learning method that can perform robust and precise atom segmentation, localization, denoising, and super-resolution processing of experimental images. Despite using simulated images as training datasets, the deep-learning model can self-adapt to experimental STEM images and shows outstanding performance in atom detection and localization in challenging contrast conditions and the precision consistently outperforms the state-of-the-art two-dimensional Gaussian fit method. Taking a step further, we have deployed our deep-learning models to a desktop app with a graphical user interface and the app is free and open-source. We have also built a TEM ImageNet project website for easy browsing and downloading of the training data.

25 ENERGY STORAGE↗
DOE OSTI2023

Shadow molecular dynamics and atomic cluster expansions for flexible charge models

A shadow molecular dynamics scheme for flexible charge models is presented, where the shadow Born-Oppenheimer potential is derived from a coarse-grained approximation of range-separated density functional theory. The interatomic potential, including the atomic electronegativities and the charge-independent short-range part of the potential and force terms, are modeled by the linear atomic cluster expansion (ACE), which provides a computationally efficient alternative to many machine learning methods. The shadow molecular dynamics scheme is based on extended Lagrangian (XL) Born-Oppenheimer molecular dynamics (BOMD) [Eur. Phys. J. B 94, 164 (2021)]. XL-BOMD provides a stable dynamics, while avoiding the costly computational overhead associated with solving an all-to-all system of equations, which normally is required to determine the relaxed electronic ground state prior to each force evaluation. To demonstrate the proposed shadow molecular dynamics scheme for flexible charge models using the atomic cluster expansion, we emulate the dynamics generated from self-consistent charge density functional tight-binding (SCC-DFTB) theory using a second-order charge equilibration (QEq) model. The charge-independent potentials and electronegativities of the QEq model are trained for a supercell of uranium oxide (UO2) and a molecular system of liquid water. The combined ACE + XL-QEq dynamics are stable over a wide range of temperatures both for the oxide and the molecular systems, and provide a precise sampling of the Born-Oppenheimer potential energy surfaces. Accurate ground Coulomb energies are produced by the ACE-based electronegativity model during an NVE simulation of UO 2 , predicted to be within 1 meV of those from SCC-DFTB on average during comparable simulations.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Hydrogen Localization and Cluster Formation in α-Zr from First-Principles Investigations

We report alpha-zirconium (α-Zr) is a hydrogen atom host material used in nuclear energy and semiconducting applications due to Zr's excellent properties such as corrosion resistance, low thermal neutrons cross-section, and thermodynamically favorable interstitial sequestering of H atoms. Herein we use density functional theory simulations to systematically analyze the initial stages of H insertion in the Zr matrix, and determine optimal hydrogen localization, distribution, and clustering tendencies from a thermodynamics and kinetics perspective. Our results suggest that H occupation of tetrahedral sites is strongly favored, consistent with previous experimental and theoretical studies. Further, a cooperative effect in H localization is shown where H atoms favor clustering. The H pair is found to be the most stable by occupying tetrahedral sites with pairs at second nearest-neighbor positions (TTn2). Among the four H atom clusters, the most favorable configuration has two TTn2 pairs forming "box " or "zig-zag" shaped-cluster with the pairs separated by 3.03 or 3.25 Å, respectively. Nudged elastic band simulations suggest that the formation of TTn2 is facile and is limited by the small diffusion barrier of the monomer of less than 0.1 eV. Further, the formation routes for the 4H atom clusters are also presented. The current study can serve as a foundation to systematically model H atom clustering in metals and alloys.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Local Structure and Electronic State of Atomically Dispersed Pt Supported on Nanosized CeO 2

Single atom catalysts (SACs) have shown high activity and selectivity in a growing number of chemical reactions. Many efforts aimed at unveiling the structure–property relationships underpinning these activities and developing synthesis methods for obtaining SACs with the desired structures are hindered by the paucity of experimental methods capable of probing the attributes of local structure, electronic properties, and interaction with support—features that comprise key descriptors of their activity. Here in this work, we describe a combination of experimental and theoretical approaches that include photon and electron spectroscopy, scattering, and imaging methods, linked by density functional theory calculations, for providing detailed and comprehensive information on the atomic structure and electronic properties of SACs. This characterization toolbox is demonstrated here using a model single atom Pt/CeO 2 catalyst prepared via a sol–gel-based synthesis method. Isolated Pt atoms together with extra oxygen atoms passivate the (100) surface of nanosized ceria. A detailed picture of the local structure of Pt nearest environment emerges from this work involving the bonding of isolated Pt 2+ ions at the hollow sites of perturbed (100) surface planes of the CeO 2 support, as well as a substantial (and heretofore unrecognized) strain within the CeO 2 lattice in the immediate vicinity of the Pt centers. The detailed information on structural attributes provided by our approach is the key for understanding and improving the properties of SACs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1992

SiO(X) coatings for atomic oxygen protection of polyimide Kapton in low earth orbit

Sputter-deposited SiO(X) (where X between 1.9 and 2.0) thin film coatings have been found to be durable to atomic oxygen. Such coatings will be used to protect polyimide Kapton photovoltaic array blankets from atomic oxygen attack in low earth orbit (LEO) on the Space Station Freedom (SSF). Monte Carlo modeling of atomic oxygen attack at defect sites in protected Kapton exposed in laboratory RF plasma ashers and on solar tracking photovoltaic arrays in space has been conducted to enable understanding of degradation processes relevant to the durability of the SSF solar array blanket. SiO(X) protective coating performance data from RF plasma asher tests will be presented, along with Monte Carlo modeling considerations, to enable the projection of in-space durability of the SSF solar array blankets based on ground laboratory test results.

Banks, Bruce A.↗
NASA NTRS1980

The ultraviolet dayglow. I - Far UV emissions of N and N2

Far ultraviolet rocket spectra of N I and N2 dayglow emissions have been analyzed by using AE-E photoelectron spectra, laboratory-measured excitation cross sections, and photochemical models of atomic nitrogen. A self-consistent picture of both optically thick and thin emission features is found by using a model in which the principal production mechanism for N I 1200-A and 1493-A photons is photodissociative excitation of N2. The aeronomic data require that 50-70% of the excited 4 P atoms produced dissociatively have velocities within the Doppler core of the ambient nitrogen atoms, contrary to the expectation that those atoms are produced with large excess kinetic energy. The derived atomic nitrogen density has a maximum density of 2.7 x 10 to the 7th per cu cm at 170 km, a value that is within 40% of that from recent models of odd nitrogen photochemistry.

Meier, R. R.↗
DOE OSTI2015

Effects of local field and inherent strain in reflectance anisotropy spectra of A{sup III}B{sup V} semiconductors with naturally oxidized surfaces

Reflectance anisotropy (RA) spectra of naturally oxidized (001) surfaces of GaAs and InAs crystals are measured for photon energies from 1.5 up to 5.5 eV. The differential high-accuracy RA spectra reveal features substantially different from those caused by either a reconstruction of clean surface or a built-in near-surface electric field. Models of atomic structure with anisotropic transition layers of excess arsenic atoms specific for GaAs(001)/oxide and InAs(001)/oxide interfaces are proposed. In conformity with these models, a general theory of reflectance anisotropy is developed for semiconductor/oxide interfaces within the Green's function technique. The theory takes into account the combined effect of local field due to interface dipoles and of intrinsic near-surface strain of the crystal. Measured RA spectra are analyzed in the model of valence-bond dipoles occupying a rectangular lattice in a multilayer medium. Comparing the measured and calculated spectra, we conclude that RA spectra of oxidized GaAs(001) and InAs(001) surfaces are simultaneously influenced by interface and near-surface anisotropies. The former is responsible for the broad-band spectral features which are associated with polarizability of the valence bonds attached to As atoms at the crystal/oxide interface. The near-surface anisotropy is due to inherent uniaxial straining the near-surface region of crystal. The effect of strain on RA spectra is experimentally and theoretically substantiated for GaAs crystal wafers undergone a uniaxial applied stress. Basically, this work results in the following. It establishes the physical nature of different levels of RA spectra observed in a majority of papers, but never analyzed. It demonstrates how the studied features of RA spectra could be applied for optical characterization of strained interfaces and atomic layers.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Atomic-scale dynamics of a model glass-forming metallic liquid: Dynamical crossover, dynamical decoupling, and dynamical clustering

The phase behavior of multi-component metallic liquids is exceedingly complex because of the convoluted many-body and many-elemental interactions. Herein, we present systematic studies of the dynamic aspects of such a model ternary metallic liquid Cu 40 Zr 51 Al 9 using molecular dynamics simulation with embedded atom method. We observed a dynamical crossover from Arrhenius to super-Arrhenius behavior in the transport properties (diffusion coefficient, relaxation times, and shear viscosity) bordered at T x ~1300K. Unlike in many molecular and macromolecular liquids, this crossover phenomenon occurs in the equilibrium liquid state well above the melting temperature of the system (T m ~ 900K), and the crossover temperature is roughly twice of the glass-transition temperature (T g ). Below T x , we found the elemental dynamics decoupled and the Stokes-Einstein relation broke down, indicating the onset of heterogeneous spatially correlated dynamics in the system mediated by dynamic communications among local configurational excitations. To directly characterize and visualize the correlated dynamics, we employed a non-parametric, unsupervised machine learning technique and identified dynamical clusters of atoms with similar atomic mobility. The revealed average dynamical cluster size shows an accelerated increase below T x and mimics the trend observed in other ensemble averaged quantities that are commonly used to quantify the spatially heterogeneous dynamics such as the non-Gaussian parameter and the four-point correlation function.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1973

Cas A X-ray spectrum: Evidence for iron line emission

A sensitive measurement by rocket borne detectors of the X-ray flux from Cas A has revealed a steep continuum and a broad spectral feature in the region where line radiation from iron nuclei would be expected. The flux in this feature is .0122 plus or minus .0017 photons/sq cm/s: the total energy flux from 2 to 10 KeV is 1.02 x 10 to the minus 9th power ergs/sq cm/s. The presence of broad iron lines is consistent with a model in which approximately 13 MeV/nucleon iron nuclei charge exchange with surrounding interstellar oxygen and other heavy atoms. The model suggests that a substantial fraction of the energy from the outburst has gone into low energy cosmic rays which produce the observed HII region surrounding the remnant.

Serlemitsos, P. J.↗
DOE OSTI2025

Quantum mechanical dataset of 836k neutral closed-shell molecules with up to 5 heavy atoms from C, N, O, F, Si, P, S, Cl, Br

Abstract We introduce the Vector-QM24 (VQM24) dataset comprehensively covering all possible neutral closed-shell small organic and inorganic molecules with up to five heavy (p-block) atoms: C, N, O, F, Si, P, S, Cl, Br. All valid stoichiometries, Lewis-rule-consistent graphs, and stable conformers (identified via GFN2-xTB) were enumerated combinatorially, yielding 577k conformational isomers spanning 258k constitutional isomers and 5,599 unique stoichiometries. DFT (ωB97X-D3/cc-pVDZ) optimizations were performed for all, and diffusion quantum Monte Carlo (DMC@PBE0(ccECP/cc-pVQZ)) energies are provided for 10,793 lowest-energy conformers with up to 4 heavy atoms. VQM24 includes structures, vibrational modes, rotational constants, thermodynamic properties (Gibbs free energies, enthalpies, ZPVEs, entropies, heat capacities), and electronic properties such as atomization, electron interaction, exchange-correlation, dispersion energies, multipole moments (dipole to hexadecapole), alchemical potentials, Mulliken charges, and wavefunctions. Machine learning models of atomization energies on this dataset reveal significantly higher complexity than QM9, with none achieving chemical accuracy. VQM24 offers a rigorous, high-fidelity benchmark for evaluating quantum machine learning models.

Science & Technology - Other Topics↗
DOE OSTI2019

Bridging the Homogeneous-Heterogeneous Divide: Modeling Spin for Reactivity in Single Atom Catalysis

Single atom catalysts (SACs) are emergent catalytic materials that have the promise of merging the scalability of heterogeneous catalysts with the high activity and atom economy of homogeneous catalysts. Computational, first-principles modeling can provide essential insight into SAC mechanism and active site configuration, where the sub-nm-scale environment can challenge even the highest-resolution experimental spectroscopic techniques. Nevertheless, the very properties that make SACs attractive in catalysis, such as localized d electrons of the isolated transition metal center, make them challenging to study with conventional computational modeling using density functional theory (DFT). For example, Fe/N-doped graphitic SACs have exhibited spin-state dependent reactivity that remains poorly understood. However, spin-state ordering in DFT is very sensitive to the nature of the functional approximation chosen. In this work, we develop accurate benchmarks from correlated wavefunction theory (WFT) for relevant octahedral complexes. We use those benchmarks to evaluate optimal DFT functional choice for predicting spin state ordering in small octahedral complexes as well as models of pyridinic and pyrrolic nitrogen environments expected in larger SACs. Using these guidelines, we determine Fe/N-doped graphene SAC model properties and reactivity as well as their sensitivities to DFT functional choice. Finally, we conclude with broad recommendations for computational modeling of open-shell transition metal single-atom catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗