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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

Distilling nanoscale heterogeneity of amorphous silicon using tip-enhanced Raman spectroscopy (TERS) via multiresolution manifold learning

Abstract Accurately identifying the local structural heterogeneity of complex, disordered amorphous materials such as amorphous silicon is crucial for accelerating technology development. However, short-range atomic ordering quantification and nanoscale spatial resolution over a large area on a-Si have remained major challenges and practically unexplored. We resolve phonon vibrational modes of a-Si at a lateral resolution of <60 nm by tip-enhanced Raman spectroscopy. To project the high dimensional TERS imaging to a two-dimensional manifold space and categorize amorphous silicon structure, we developed a multiresolution manifold learning algorithm. It allows for quantifying average Si-Si distortion angle and the strain free energy at nanoscale without a human-specified physical threshold. The multiresolution feature of the multiresolution manifold learning allows for distilling local defects of ultra-low abundance (< 0.3%), presenting a new Raman mode at finer resolution grids. This work promises a general paradigm of resolving nanoscale structural heterogeneity and updating domain knowledge for highly disordered materials.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Chemical and structural evolutions of Li–Mn-rich layered electrodes at different current densities

Although the two active redox centers in Li-rich cathodes, including the anionic and cationic contributions, can enable Li-ion batteries to achieve outstanding specific energy, their behaviors at different current densities have not been clarified. In this report we provide a comparative study of transition metals (TMs) and oxygen redox activities by directly accessing their oxidation states in Li-rich materials operated at very different current rates. Our data reveal that the oxidation of oxygen in the near-surface region is at the same level for electrodes cycled with a wide range of current rates, indicating a reaction gradient of lattice oxygen redox reactions. The oxidation process of lattice oxygen is found to be dynamically compatible with that of the TMs. Combining the results of first principles calculations and complementary experimental findings, we propose a detailed mechanism of structural distortion from octahedral Li to tetrahedral Li and the role of oxygen vacancy in Li + diffusion. It is found that fast delithiation occurring at high current densities can easily cause local structural transformation, leading to a limited Li + diffusion rate and consequently suppressing rate capability.

25 ENERGY STORAGE↗
DOE OSTI2021

Dimensional Control of Octahedral Tilt in SrRuO 3 via Infinite-Layered Oxides

Manipulation of octahedral distortion at atomic scale is an effective means to tune the ground states of functional oxides. Previous work demonstrates that strain and film thickness are variable parameters to modify the octahedral parameters. However, selective control of bonding geometry by structural propagation from adjacent layers is rarely studied. Here we propose a new route to tune the ferromagnetism in SrRuO 3 (SRO) ultrathin layers by oxygen coordination of adjacent SrCuO 2 (SCO) layers. The infinite-layered CuO 2 exhibits a structural transformation from “planar-type” to “chain-type” with reduced film thickness. Two orientations dramatically modify the polyhedral connectivity at the interface, thus altering the octahedral distortion of SRO. The local structural variation changes the spin state of Ru and orbital hybridization strength, leading to a significant change in the magnetoresistance and anomalous Hall resistivity. Furthermore, these findings could launch investigations into adaptive control of functionalities in quantum oxide heterostructures using oxygen coordination.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Quantifying the hierarchy of structural and mechanical length scales in granular systems

Continuum modeling of granular media is made possible by the existence of a length scale at and above which grain-resolved properties can be meaningfully homogenized. Progress has been made in identifying such length scales relevant to local structural properties such as porosity. However, a systematic analysis of scales above which different mechanical properties can be homogenized has yet to emerge. Here, X-ray tomography and 3D X-ray diffraction data are examined to identify such length scales. The data was obtained in-situ in compressed granular materials with rigid and flexible confinement. The experimental data are supplemented with validated discrete element simulations which examine different system sizes and different boundary conditions. Overall, our study reveals a hierarchy in the length scales of granular solids, with lengths governing structural variables being the shortest, lengths of stress variables being intermediate, and lengths of energy dissipation being the longest. All structural and mechanical length scales obey a power law based on the theory of Geostatistics, implying that the length scales can be found by analyzing samples significantly smaller than the length scales themselves. The length scales are also found to be sensitive to boundary conditions, implying that they are extrinsic features of granular media.

36 MATERIALS SCIENCE↗
NASA NTRS1993

Global-, local-, and intermediate-scale structures in prototype spiral galaxies

The relationship between galactic spiral structure and the matter in the underlying disk constitutes one of the central problems in galactic dynamics. In Bertin et al. (1989), disk matter characterized by a low-dispersive speed is shown to be capable of playing a key role in the generation of large-scale spiral structure. In Roberts et al. (1992), this self-gravitating, low-dispersion disk matter is shown to be capable of playing an essential role in the formation of structure on local and intermediate scales. Both in computed cases where large-scale spiral structure is present and in those where it is not, the same dominant physical processes and fundamental dynamical mechanisms are active on local scales. The new perception, in which large-scale and small-scale phenomena operate somewhat independently as evidenced in the computational studies, permits a range of flocculent, multiarmed, and grand design spiral types to be simulated. In particular, grand design galaxies with ragged appearances exhibiting spurs, arm branchings, and interarm bridges in addition to the major spiral arms, similar to those often observed, can be generated.

Roberts, William W., Jr.↗
DOE OSTI2025

Observation of Topological Spin Textures in Ferrimagnetic Mn 2 − x Zn x Sb

Ferrimagnets, which have both ferromagnetic and antiferromagnetic coupling, are attracting increased attention in the realm of spintronic devices due to advantages such as ultrafast dynamics and a suppressed skyrmion Hall effect. Thus, understanding the behavior of nontrivial spin textures in ferrimagnets is crucial; however, comprehensive reports on this topic remain limited. Here, the magnetic spin textures of ferrimagnetic Mn 2 − x Zn x Sb (x = 0.85) is explored as a function of temperature and applied magnetic field. The spin textures can be tuned to a variety of states, including stripes, skyrmion bags, and a skyrmion lattice. Chiral Néel-type magnetic structures are visualized using Lorentz transmission electron microscopy. Mn(I) ions are slightly shifted toward the Sb sites, which may be due to a strong electrostatic interaction between Mn and Sb ions. This local structural distortion breaks the inversion symmetry and introduces an effective Dzyaloshinkii–Moriya interaction. This work thus provides a pathway to use doping and heterogeneity in a ferrimagnet to control and generate chiral nontrivial spin textures.

Mn ion displacement↗
DOE OSTI2026

Pressure-Driven Helium Insertion for Structural Stability of CH 3 NH 3 PbBr 3 Hybrid Perovskites

Organic−inorganic metal halide perovskites (MHPs) have garnered significant attention due to their outstanding performance in optoelectronic devices, but they are prone to degradation through a variety of pathways. High-pressure studies are being used to understand the mechanical and structural stability of MHPs and investigate new methods for improving these. In this study, we map the high-pressure, low-temperature structural phase diagram of CH 3 NH 3 PbBr 3 (MAPbBr 3 ) between 15−300 K and up to 1.5 GPa. We first compare the temperature and pressure effects on the global and local structures of MAPbBr 3 using synchrotron X-ray diffraction (XRD) and extended X-ray absorption fine structure (EXAFS), respectively, and find evidence of PbBr 6 octahedral distortion. Our results also suggest that He inserts into the MAPbBr 3 structure. The thermodynamics of He insertion into MAPBHe x are calculated to be plausible at room temperature for x ≤ 1 and P = 1−3 GPa and shown to stabilize higher-symmetry phases. This phenomenon increases the fitted bulk modulus of MAPbBr 3 . Structural stabilization by inert atom insertion is proposed as a method to improve the mechanical robustness of MHPs and other soft hybrid materials.

Diffraction↗
DOE OSTI2024

Defect-Limited Mobility and Defect Thermochemistry in Mixed A-Cation Tin Perovskites: (CH3NH3)1-xCsxSnBr3

Hybrid organic-inorganic semiconductors crystallizing in the perovskite structure present a significant opportunity for realizing defect-tolerant semiconductors. In this work, we examine the solid solution, (CH3NH3)1-xCsxSnBr3, and identify the thermochemistry dictating the intrinsic carrier concentrations and how local structural distortions influences this electronic behavior. This family of compounds exhibits the expected systematic trend in decreasing optical gap with the cesium to methylammonium A-site mixing ratio, x, in the visible region. However, the carrier mobility, as determined from time-resolved microwave conductivity measurements, trends opposite to that expected from first-principles calculations combined with Boltzmann scattering theory calculations of the carrier mobility. We propose that this is a result of increasing carrier scattering with x in (CH3NH3)1-xCsxSnBr3 due to a significant increase in the carrier density with x. By examining the dependence of the carrier density as a function of x, we infer the compositional-dependence of the average enthalpy and nonconfigurational entropy per defect. While diffraction reveals a cubic aristotypic perovskite structure as a function of x at room temperature, the pair distribution functions obtained from synchrotron X-ray total scattering from these materials are better described by symmetry-adapted displacement modes of the Pm3m crystal structure, which we attribute to a large degree of anharmonic dynamics of the atom positions. This analysis shows that CH3NH3+-rich compositions retain mostly linear Sn-Br-Sn bonding environments through the displacements, while Cs+-rich compositions lead to more significantly bent Sn-Br-Sn environments. We propose that these bent bonding arrangements in Cs-rich compositions yield a higher propensity for defect formation. This also provides a rationale for carrier trapping that gives rise to anomalous microwave transients. Together, these results provide insight into the structure-dynamics-properties relationships in this highly anharmonic system with high amplitude atomic motions and low defect formation energies.

defect thermochemistry↗
DOE OSTI2025

Structure of Iridium Oxides and Their Oxygen Evolution Electrocatalysis in Acidic Media

Proton exchange membrane water electrolyzers (PEMWEs) have emerged as one of the most promising technologies for the large-scale production of clean hydrogen. Gigawatt scale deployment of PEMWEs requires substantial reduction in the loading of iridium (Ir), which is one of the most expensive and rarest elements. Substantial reduction in Ir loading calls for the development of innovative Ir-based anodes, which requires a clear understanding of how iridium oxides accelerate the sluggish oxygen evolution reaction (OER) in acidic media. Herein, we studied the structure and OER electrocatalysis of three representative iridium oxides ─ hydrous, amorphous, and rutile ─ by employing a combination of physicochemical and electrochemical characterization. Additionally, we found that the hydrous iridium oxide had a different local structure of IrO 6 octahedra and a superior OER intrinsic activity compared with the other two, and that the OER activities of all three types decreased with decreasing pH of acidic solution. We proposed that the OER process of these iridium oxides is limited by water nucleophilic attack on the OER intermediate oxygenated adsorbates. Based on this mechanism, we attributed the superior OER activity of hydrous iridium oxides to their longer Ir–O bonds and the pH-dependent OER activity of iridium oxides to the pH-dependent oxidation of Ir.

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

Evidence for pseudo–Jahn-Teller distortions in the charge density wave phase of 1$\textit{T}-\text{TiSe}_2$

Here, the charge density wave (CDW) instability in 1$\textit{T}-\text{TiSe}_2$ is revisited to investigate its electronic and structural origins using angle resolved photoemission spectroscopy (ARPES), neutron diffraction, and density functional theory (DFT) calculations. The evidence for Jahn-Teller (JT)-like distortions in the CDW state is provided from the local structure analysis that shows splitting of the Ti-Se bonds into short and long. The magnitude of the split is inconsistent with the commonly accepted Di Salvo model for the structural distortions in the CDW phase. From the APRES data, it is deduced that a nontrivial temperature-dependent energy shift of the Se $4\textit{p}$ valence bands occurs, but is absent for the Ti $3\textit{d}$ conduction bands. Collectively, these observations suggest that a JT-like mechanism is most likely central to the CDW instability in 1$\textit{T}-\text{TiSe}_2$.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Temperature-Dependent Properties of Molten Li 2 BeF 4 Salt Using Ab Initio Molecular Dynamics

Molten lithium tetrafluoroberyllate (Li 2 BeF 4 ) salt, also known as FLiBe, with a 2:1 mixture of LiF and BeF 2 is being proposed as a coolant and solvent in advanced nuclear reactor designs, such as the molten salt reactor or the fluoride salt cooled high-temperature reactor. We present the results on the structure and properties of FLiBe over a wide range of temperatures, 0–2000 K, from high-throughput ab initio molecular dynamics simulation using a supercell model of 504 atoms. The variations in the local structures of solid and liquid FLiBe with temperature are discussed in terms of a pair distribution function, coordination number, and bond angle distribution. The temperature-dependent electronic structure and optical and mechanical properties of FLiBe are calculated. The optical and mechanical property results are reported for the first time. The results above and below the melting temperature (~732 K) are compared with the experimental data and with data for crystalline FLiBe. The electronic structure and interatomic bonding results are discussed in correlation with the mechanical strength. A novel concept of total bond order density (TBOD), an important quantum mechanical parameter, is used to characterize the internal cohesion and strength in the simulated models. The results show a variation in the rate of change in properties in solid and liquid phases with anomalous behavior across the melting region. The observed trend is the decrease in mechanical strength, band gap, and TBOD in a nonlinear fashion as a function of temperature. The refractive index shows a surprising minimum at 850 K, among the tested temperatures, which lies above the melting point. These findings provide a new platform to understand the interplay between the temperature-dependent structures and properties of FLiBe salt.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Gaussian approximation potential for amorphous Si : H

Hydrogenation of amorphous silicon (a–Si : H) is critical for reducing defect densities, passivating midgap states and surfaces, and improving photoconductivity in silicon-based electro-optical devices. Modeling the atomic-scale structure of this material is critical to understanding these processes, which in turn is needed to describe c–Si/a–Si : H heterojunctions that are at the heart of modern solar cells with world-record efficiency. Density functional theory (DFT) studies achieve the required high accuracy but are limited to moderate system sizes of 100 atoms or so by their high computational cost. Simulations of amorphous materials have been hindered by this high cost because large structural models are required to capture the medium-range order that is characteristic of such materials. Empirical potential models are much faster, but their accuracy is not sufficient to correctly describe the frustrated local structure. Data-driven, machine-learned interatomic potentials have broken this impasse and have been highly successful in describing a variety of amorphous materials in their elemental phase. Here, we extend the Gaussian approximation potential (GAP) for silicon by incorporating the interaction with hydrogen, thereby significantly improving the degree of realism with which amorphous silicon can be modeled. We show that our Si : H GAP enables the simulation of hydrogenated silicon with an accuracy very close to DFT but with computational expense and run times reduced by several orders of magnitude for large structures. Here, we demonstrate the capabilities of the Si : H GAP by creating models of hydrogenated liquid and amorphous silicon and showing that their energies, forces, and stresses are in excellent agreement with DFT results, and their structure as captured by bond and angle distributions are in agreement with both DFT and experiments.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Doping topological Dirac semimetal with magnetic impurities: Electronic structure of Mn-doped Cd 3 ⁢As 2

The prospect of transforming a Dirac topological semimetal (TSM) into a Weyl TSM phase, following doping by magnetic impurities, is central to TSM applications. The magnetic field from polarized 𝑑 levels of magnetic impurities produces a field with a sharp local structure. To what extent magnetic impurities act in the same manner as an applied field and what are the effects of such a field on the electronic structure of a Dirac TSM are the subject of this paper. We present electronic structure calculations of bulk Cd 3 ⁢As 2 with substitutional doping of Mn impurities in the dilute alloy range. Quasiparticle 𝐺⁡𝑊 (QS⁢𝐺⁡𝑊) ab initio electronic structure calculations are used in conjunction with 𝑘 · 𝑝 model Hamiltonian calculations. As expected, we observe the splitting of the Dirac points into pairs of Weyl points following the doping with Mn. We also show that the electronic structure of Mn-doped Cd 3⁢ As 2 can be emulated by the electronic structure of pristine Cd 3⁢ As 2 with an appropriate external magnetic field. Some properties of the conductivity of bulk Cd 3 ⁢As 2 for different magnetic field orientations are also investigated. Our results inform future opportunities for unique device functionality based on band structure tuning not found in conventional magnetic Weyl TSM.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Additive Destabilization of Porous Magnesium Borohydride Framework with Core--Shell Structure

Design of interfaces with thermodynamic and kinetic specificity is of great importance for hydrogen storage from both an applied and fundamental perspective. Here, in order to destabilize the metal hydride and protect the dehydrogenated products from oxidizing, a unique core-shell structure of porous Mg(BH4)2-based framework with a thin layer (no more than 5 nm) of MgCl2 additives on the surface, has been proposed and synthesized via a wet-chemical method. The local structure and electronic state of the present complex system are systematically investigated to understand the correlation between the distribution of additives and dehydrogenation property of Mg(BH4)2. A significant improvement is achieved for hydrogen desorption with chlorides: initial hydrogen release from MgCl2 decorated ..gamma..-phase Mg(BH4)2 particles commences at 100 °C and reaches a maximum of 9.4 wt% at 385 °C. Besides the decreased decomposition temperature, an activation barrier of about 76.4 kJ mol-1 lower than that of Mg(BH4)2 without MgCl2 is obtained. Moreover, MgCl2 decoration can also prevent the whole decomposed system (both Mg- and B- elements) from oxidizing, which is a necessary condition to reversibility.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2023

Brominated lipid probes expose structural asymmetries in constricted membranes

Lipids in biological membranes are thought to be functionally organized, but few experimental tools can probe nanoscale membrane structure. Using brominated lipids as contrast probes for cryo-EM and a model ESCRT-III membrane-remodeling system composed of human CHMP1B and IST1, we observed leaflet-level and protein-localized structural lipid patterns within highly constricted and thinned membrane nanotubes. These nanotubes differed markedly from protein-free, flat bilayers in leaflet thickness, lipid diffusion rates and lipid compositional and conformational asymmetries. Simulations and cryo-EM imaging of brominated stearoyl-docosahexanenoyl-phosphocholine showed how a pair of phenylalanine residues scored the outer leaflet with a helical hydrophobic defect where polyunsaturated docosahexaenoyl tails accumulated at the bilayer surface. Combining cryo-EM of halogenated lipids with molecular dynamics thus enables new characterizations of the composition and structure of membranes on molecular length scales.

59 BASIC BIOLOGICAL SCIENCES↗
NASA NTRS2003

A Mechanism for Recent Production of Liquid Water on Mars

Though Mars is a cold, dry planet, with respect to the thermal stability of liquid water at low altitudes it is not terribly different from comparably cold places on Earth. In dry air such water would evaporate faster on Mars, at a rate comparable to a 60 C hot spring on Earth, but the heat loss associated with that evaporation would be mitigated by the poor thermal convection in the thin Martian air. Even at higher altitudes where the atmospheric pressure does not reach the triple point of water, liquid water might theoretically exist in a low-vapor pressure form such as wet soil, in a briny solution, or simply under a layer of dust or snow. The theoretical stability of liquid water does not suggest its occurrence, either on Mars or in Antarctica. In fact, global models have suggested that locations capable of providing sufficient heat for melting are, precisely for that reason, too dry for water to be present. However, the temperature of irregular local structures such as trenches or craters can be markedly warmer than those of the uniform surfaces of global models. The work described here suggests a plausible scenario in which seasonal liquid water might be produced locally, in sheltered locations, through a process of condensation, cold-trapping, buffering, and melting. While the amounts produced in the present climate would be small, copious amounts of meltwater may have been produced at other phases of the orbital cycle, as recently as 20,000 years ago.

Hecht, M. H.↗
NASA NTRS2006

Boundary Layer Transition Results From STS-114

The tool for predicting the onset of boundary layer transition from damage to and/or repair of the thermal protection system developed in support of Shuttle Return to Flight is compared to the STS-114 flight results. The Boundary Layer Transition (BLT) Tool is part of a suite of tools that analyze the aerothermodynamic environment of the local thermal protection system to allow informed disposition of damage for making recommendations to fly as is or to repair. Using mission specific trajectory information and details of each damage site or repair, the expected time of transition onset is predicted to help determine the proper aerothermodynamic environment to use in the subsequent thermal and stress analysis of the local structure. The boundary layer transition criteria utilized for the tool was developed from ground-based measurements to account for the effect of both protuberances and cavities and has been calibrated against flight data. Computed local boundary layer edge conditions provided the means to correlate the experimental results and then to extrapolate to flight. During STS-114, the BLT Tool was utilized and was part of the decision making process to perform an extravehicular activity to remove the large gap fillers. The role of the BLT Tool during this mission, along with the supporting information that was acquired for the on-orbit analysis, is reviewed. Once the large gap fillers were removed, all remaining damage sites were cleared for reentry as is. Post-flight analysis of the transition onset time revealed excellent agreement with BLT Tool predictions.

Berry, Scott A.↗