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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 1,189 records · Page 66
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Magnetotransport properties of a few-layer graphene-ferromagnetic metal junctions in vertical spin valve devices

Magnetotransport properties were studied for the vertical spin valve devices with two junctions of permalloy electrodes and a few-layer graphene interlayer. The graphene layer was directly grown on the bottom electrode by chemical vapor deposition. X-ray photoelectron spectroscopy showed that the permalloy surface fully covered with a few-layer graphene is kept free from oxidation and contamination even after dispensing and removing photoresist. This enabled fabrication of the current perpendicular to plane spin valve devices with a well-defined interface between graphene and permalloy. Spin-dependent electron transport measurements revealed a distinct spin valve effect in the devices. The magnetotransport ratio was 0.8% at room temperature and increased to 1.75% at 50 K. Linear current-voltage characteristics and resistance increase with temperature indicated that ohmic contacts are realized at the relevant interfaces.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Measurement of valence-band offset at native oxide/BaSi{sub 2} interfaces by hard x-ray photoelectron spectroscopy

Undoped n-type BaSi{sub 2} films were grown on Si(111) by molecular beam epitaxy, and the valence band (VB) offset at the interface between the BaSi{sub 2} and its native oxide was measured by hard x-ray photoelectron spectroscopy (HAXPES) at room temperature. HAXPES enabled us to investigate the electronic states of the buried BaSi{sub 2} layer non-destructively thanks to its large analysis depth. We performed the depth-analysis by varying the take-off angle (TOA) of photoelectrons as 15°, 30°, and 90° with respect to the sample surface and succeeded to obtain the VB spectra of the BaSi{sub 2} and the native oxide separately. The VB maximum was located at −1.0 eV from the Fermi energy for the BaSi{sub 2} and −4.9 eV for the native oxide. We found that the band bending did not occur near the native oxide/BaSi{sub 2} interface. This result was clarified by the fact that the core-level emission peaks did not shift regardless of TOA (i.e., analysis depth). Thus, the barrier height of the native oxide for the minority-carriers in the undoped n-BaSi{sub 2} (holes) was determined to be 3.9 eV. No band bending in the BaSi{sub 2} close to the interface also suggests that the large minority-carrier lifetime in undoped n-BaSi{sub 2} films capped with native oxide is attributed not to the band bending in the BaSi{sub 2}, which pushes away photogenerated minority carriers from the defective surface region, but to the decrease of defective states by the native oxide.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Orienting Strained Interfaces designed to Direct Energy Flow (Final Technical Report)

This proposal aims to establish a transformative paradigm for oxide heterostructures with an exceptionally large number of interfaces designed to direct energy flow through controlled interface orientation, enabling fast ion transport. A primary focus is on unveiling the key role of interfacial strain in oxygen ion migration at low temperatures. The central challenge is to create, understand, utilize self-assembled vertical heteroepitaxial nanostructures with the goal of obtaining and understanding fast ion transport properties by modulating interfacial strain. The specific objectives are: (1) to synthesize multilayer thin films and vertical heteroepitaxial nanostructures with fluorite Gd-doped CeO 2 (GDC) and bixbyite RE 2 O 3 (RE = Y and Sm), (2) to evaluate the interfacial strain states under various temperatures and ambient conditions, (3) to understand the effect of interfacial strain on ionic conductivity of the proposed nanostructures, (4) to understand the three-dimensional (3D) atomic structure of the proposed material design and interface phenomena at the atomic scale.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Unveiling the nucleation and growth of Zr oxide precipitates in internally oxidized Nb3Sn superconductors

We report on atomic-scale analyses of nucleation and growth of Zr oxide precipitates and the microstructural evolution of internally oxidized Nb3Sn wires for high-field superconducting magnet applications, utilizing atom probe tomography (APT), transmission electron microscopy (TEM), and first-principles calculations. APT analyses reveal that oxygen and zirconium are already segregated at grain boundaries (GBs) in the unreacted Nb-1Zr-4Ta (at%) alloy prior to forming Nb3Sn through reacting the Nb alloy with Sn and SnO2. After forming Nb3Sn, Zr oxide precipitates nucleate both at the Nb3Sn/Nb heterophase interfaces and in the Nb3Sn grains, driven by the small solubilities of Zr and O in Nb3Sn compared to their value in Nb. A high number density (Nv) of Zr oxide nanoprecipitates is observed in the Nb3Sn layers, ∼10 23 m −3 , with a mean diameter <10 nm for a heat treatment at 625 °C. Quantitative APT and TEM analyses of the Zr oxide precipitates in the reacted Nb3Sn layers elucidate details of the nucleation, growth, and coarsening processes of the Zr oxide precipitates in Nb3Sn. First-principles calculations and classical nucleation theory are employed to study the nucleation of Zr oxide precipitates in Nb3Sn and to estimate the maximum energy barrier and critical radius for nucleation. Our research unveils the kinetic pathways for nucleation and growth of Zr oxide precipitates and the microstructural evolution of Nb3Sn layers, which helps to understand and improve the superconducting properties of internally oxidized Nb3Sn wires for use in high-field superconducting magnets. •We investigated the nucleation and growth of Zr oxide nanoprecipitates in Nb3Sn superconductors for magnet applications.•APT and TEM analyses reveals the nucleation and growth process of Zr oxide precipitates in Nb3Sn layers.•Classical nucleation theory with DFT is employed to describe the nucleation process of Zr oxide precipitates in Nb3Sn.•We find that the interfacial reactions at Nb/Nb3Sn interface play a critical role in the nucleation of Zr oxide precipitates.•Current study provides a pathway to improve the properties of internally oxidized Nb3Sn superconducting wires.

43 PARTICLE ACCELERATORS↗
DOE OSTI2016

Microstructure evolution of a dissimilar junction interface between an Al sheet and a Ni-coated Cu sheet joined by magnetic pulse welding

An Al sheet and a Ni-coated Cu sheet were lap joined by using magnetic pulse welding (MPW). Tensile tests were performed on the joined sheets, and a good lap joint was achieved at a discharge energy of > 0.9 kJ. The weld interface exhibited a wavy morphology and an intermediate layer along the weld interface. Microstructure observations of the intermediate layer revealed that the Ni coating region consisted of a Ni–Al binary amorphous alloy and that the Al sheet region contained very fine Al nanograins. Ni fragments indicative of unmelted residual Ni from the coating were also observed in parts of the intermediate layer. Formation of these features can be attributed to localize melting and a subsequent high rate cooling of molten Al and Ni confined to the interface during the MPW process. In the absence of an oxide film, atomic-scale bonding was also achieved between the intermediate layer and the sheet surfaces after the collision. MPW utilises impact energy, which affects the sheet surfaces. From the obtained results, good lap joint is attributed to an increased contact area, the anchor effect, work hardening, the absence of an oxide film, and suppressed formation of intermetallic compounds at the interface. - Highlights: •Good lap joint of an Al sheet and a Ni-coated Cu sheet was achieved by using magnetic pulse welding. •A Ni–Al binary amorphous alloy was formed as an intermediate layer at weld interface. •Atomic-scale bonding was achieved between the intermediate layer and the sheet surfaces.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Enhancement of SOFC Cathode Electrochemical Performance Using Multi-Phase Interfaces

This work explored the use of oxide heterostructures for enhancing the catalytic and degradation properties of solid oxide fuel cell (SOFC) cathode electrodes. We focused on heterostructures of Ruddlesden-Popper and perovskite phases. Building on previous work showing enhancement of the Ruddlesden-Popper (La,Sr) 2 CoO 4 / perovskite (La,Sr)CoO 3 heterostructure compared to pure (La,Sr)CoO 3 we explored the application of related heterostructures of Ruddlesden-Popper phases on perovskite (La,Sr)(Co,Fe)O 3 . Our approaches included thin-film electrodes, physical and electrochemical characterization, elementary reaction kinetics modeling, and ab initio simulations. We demonstrated that Sr segregation to surfaces is likely playing a critical role in the performance of (La,Sr)CoO 3 and (La,Sr)(Co,Fe)O 3 and that modification of this Sr segregation may be the mechanism by which Ruddlesden-Popper coatings enhance performances. We determined that (La,Sr)(Co,Fe)O 3 could be enhanced in thin films by about 10× by forming a heterostructure simultaneously with (La,Sr) 2 CoO 4 and (La,Sr)CoO 3 . We hope that future work will develop this heterostructure for use as a bulk porous electrode.

25 ENERGY STORAGE↗
DOE OSTI2022

A computational pipeline to generate a synthetic dataset of metal ion sorption to oxides for AI/ML exploration

The charged mineral/electrolyte interfaces are ubiquitous in the surface and subsurface–including the surroundings of the geological disposal sites for radioactive waste. Therefore, understanding how ions interact with charged surfaces is critically important for predicting radionuclide mobility in the case of waste leakage. At present, the Surface Complexation Models (SCMs) are the most successful thermodynamic frameworks to describe ion retention by mineral surfaces. SCMs are interfacial speciation models that account for the effect of the electric field generated by charged surfaces on sorption equilibria. These models have been successfully used to analyze and interpret a broad range of experimental observations including potentiometric and electrokinetic titrations or spectroscopy. Unfortunately, many of the current procedures to solve and fit SCM to experimental data are not optimal, which leads to a non-transferable or non-unique description of interfacial electrostatics and consequently of the strength and extent of ion retention by mineral surfaces. Recent developments in Artificial Intelligence (AI) offer a new avenue to replace SCM solvers and fitting algorithms with trained AI surrogates. Unfortunately, there is a lack of a standardized dataset covering a wide range of SCM parameter values available for AI exploration and training–a gap filled by this study. Here, we described the computational pipeline to generate synthetic SCM data and discussed approaches to transform this dataset into AI-learnable input. First, we used this pipeline to generate a synthetic dataset of electrostatic properties for a broad range of the prototypical oxide/electrolyte interfaces. The next step is to extend this dataset to include complex radionuclide sorption and complexation, and finally, to provide trained AI architectures able to infer SCMs parameter values rapidly from experimental data. Here, we illustrated the AI-surrogate development using the ensemble learning algorithms, such as Random Forest and Gradient Boosting. These surrogate models allow a rapid prediction of the SCM model parameters, do not rely on an initial guess, and guarantee convergence in all cases.

Li, Chunhui↗
DOE OSTI2017

Quantitative comparison of bright field and annular bright field imaging modes for characterization of oxygen octahedral tilts

Octahedral tilt behavior is increasingly recognized as an important contributing factor to the physical behavior of perovskite oxide materials and especially their interfaces, necessitating the development of high-resolution methods of tilt mapping. There are currently two major approaches for quantitative imaging of tilts in scanning transmission electron microscopy (STEM), bright field (BF) and annular bright field (ABF). In this study, we show that BF STEM can be reliably used for measurements of oxygen octahedral tilts. While optimal conditions for BF imaging are more restricted with respect to sample thickness and defocus, we find that BF imaging with an aberration-corrected microscope with the accelerating voltage of 300 kV gives us the most accurate quantitative measurement of the oxygen column positions. Using the tilted perovskite structure of BiFeO 3 (BFO) as our test sample, we simulate BF and ABF images in a wide range of conditions, identifying the optimal imaging conditions for each mode. Finally, we show that unlike ABF imaging, BF imaging remains directly quantitatively interpretable for a wide range of the specimen mistilt, suggesting that it should be preferable to the ABF STEM imaging for quantitative structure determination.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Solution processed nickel oxide anodes for organic photovoltaic devices

Nickel oxide thin films have been prepared from a nickel acetylacetonate (Ni(acac)) precursor for use in bulk heterojunction organic photovoltaic devices. The conversion of Ni(acac) to NiO{sub x} has been investigated. Oxygen plasma treatment of the NiO layer after annealing at 400 °C affords solar cell efficiencies of 5.2%. Photoelectron spectroscopy shows that high temperature annealing converts the Ni(acac) to a reduced form of nickel oxide. Additional oxygen plasma treatment further oxidizes the surface layers and deepens the NiO work function from 4.7 eV for the annealed film, to 5.0 eV allowing for efficient hole extraction at the organic interface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Transmission Electron Microscopy and Electron Energy-Loss Spectroscopy Studies of Hole-Selective Molybdenum Oxide Contacts in Silicon Solar Cells

In this study, substochiometric hole-selective molybdenum oxide (MoO x ) contacts in crystalline silicon (c-Si) solar cells were investigated by a combination of transmission electron microscopy (TEM) and spatially resolved electron energy-loss spectroscopy (SR-EELS). It was observed that a ≈ 4 nm SiO x interlayer grows at the MoO x /c-Si interface during the evaporation of MoO x over a c-Si substrate. SR-EELS analyses revealed the presence of a 1.5 nm diffused MoO x /indium tin oxide (ITO) interface in both as-deposited and annealed samples. Moreover, the presence of a 1 nm thin layer with a lower oxidation state of Mo was detected at the SiO x /MoO x interface in an as-deposited state, which disappears upon annealing. Altogether, it was evident that no hole-blocking interlayer is formed at the MoO x /ITO interface during annealing and homogenization of the MoO x layer takes place during the annealing process. Furthermore, device simulations revealed that efficient hole collection is dependent on MoO x work function and that reduction in the work function of MoO x results in loss of band bending and negatively impacts hole selectivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Distance-dependent radiation chemistry: Oxidation versus hydrogenation of CO in electron-irradiated H2O/CO/H2O ices

Electron-stimulated oxidation of CO in layered H2O/CO/H2O ices was investigated with infrared reflection-absorption spectroscopy (IRAS) as function of the distance of the CO layer from the water/vacuum interface. The results show that while both oxidation and reduction reactions occur within the irradiated water films, there are distinct regions where either oxidation or reduction reactions are dominant. At depths less than ~ 15 ML, CO oxidation dominates over the sequential hydrogenation of CO to methanol (CH3OH), and CO2 is the major product of CO oxidation, consistent with previous observations. At its highest yield, CO2 accounts for ~45% of all the reacted CO. Another oxidation product is identified as the formate anion (HCO2-). In contrast, for CO buried more than ~ 35 ML below the water/vacuum interface, the CO-to-methanol conversion efficiency is close to 100%. Production of CO2 and formate are not observed for the more deeply buried CO layers, where hydrogenation dominates. Experiments with CO dosed on pre-irradiated ASW samples suggest that OH radicals are primarily responsible for the oxidation reactions. Possible mechanisms of CO oxidation, involving primary and secondary processes of water radiolysis at low temperature, are discussed. The observed distance-dependent radiation chemistry results from the higher mobility of hydrogen atoms that are created by the interaction of the 100 eV electrons with the water films. These hydrogen atoms, which are primarily created at or near the water/vacuum interface, can desorb from or diffuse into the water films, while the less-mobile OH radicals remain in the near-surface zone resulting in preferential oxidation reactions there. The diffusing hydrogen atoms are responsible for the hydrogenation reactions that are dominant for the more deeply buried CO layers.

Environmental Molecular Sciences Laboratory↗
NASA NTRS1990

Sulfur at nickel-alumina interfaces - Molecular orbital theory

Previous studies on Al-Ni alloys containing sulfur as an impurity suggest that, when S is in the interface between a metal and an oxide scale, it weakens the chemical bonding between them. This paper investigates factors responsible for this effect, using a molecular orbital theory to predict sulfur structures and electronic properties on the Ni-Al2O3 interface. It is shown that, in absence of S, the basal plane of Al2O3 will bind strongly through the Al(3+) cation surface to Ni (111). When segregated S impurity is present on the Ni surface, there are too few interfacial AlS bonds to effect good adhesion, leading to an inhibition of the oxide scale adhesion in NiCrAl alloys.

Hong, S. Y.↗
DOE OSTI2026

Investigation of coherence of niobium-based resonators enabled by a fast-sealing microwave cavity

Resonators and qubits with a niobium (Nb) base metal layer achieve some of the highest coherence times in superconducting quantum devices. The performance of such devices is often limited by loss associated with two-level systems, which are found primarily at material surfaces and interfaces. The metal-air (MA) interface is a major contributor to device loss. In this work, we develop a fast-sealing microwave cavity that enables devices to be placed under vacuum within five minutes of oxide removal, thereby significantly reducing the MA interface loss compared to common device processing and packaging approaches. Using coplanar stripline resonators, we demonstrate that devices sealed in such a cavity exhibit internal quality factors exceeding one million at single-photon power. After re-exposure to air, the devices show downward resonance frequency shifts and quality factor degradations, quantitatively consistent with a model of Nb oxide regrowth. The fast-sealing microwave cavity provides a practical and consistent method to mitigate MA interface loss and sustain high coherence in Nb devices, and establishes a controlled platform for studying metal oxide regrowth kinetics and dielectric properties, the understanding of which is critical to achieving high coherence in superconducting quantum devices.

Zhang, C. [Waterloo U., IQC; Waterloo U.]↗
DOE OSTI2025

Insight Into Sulfur‐Containing Additive to Boost Anti‐Oxidation Ability of the Ether‐Based Electrolyte for Sodium‐Ion Full Batteries

Ether-based electrolytes are considered as promising candidates for sodium-ion batteries (SIBs) due to their high ionic conductivity and good compatibility with hard carbon (HC) anode. However, they suffer from poor anti-oxidative ability with unstable cathode electrolyte interface, inducing successive electrolyte decomposition and rapid capacity fading. Herein, the sulfur-containing additive (1,3-propanediol cyclic sulfate, PCS) is introduced to boost the stability of the electrode-electrolyte interface (EEI) in ether-based electrolyte. PCS largely participates in the inner Na + sheath, causing more diglyme (G2) molecules and fewer PF 6 - anions to occupy the inner Na + solvation sheath, avoiding the decomposition of G2 molecules at high operation voltage. Moreover, PCS is beneficial for simultaneously constructing thin and robust sulfur-containing EEI on both Prussian blue (PB) cathode and HC anode, maintaining the structural stability of PB and alleviating the dissolution of transition metals. These enable PB||HC pouch cells to deliver a capacity retention of 60.3% after 400 cycles, significantly higher than the 32.1% in PCS-free electrolytes. In conclusion, this work discloses the underlying mechanism of PCS to evoke the anti-oxidation ability of ether-based electrolyte and provides a promising method for realizing advanced sodium-ion full cells.

anti-oxidation ability↗
DOE OSTI2023

Interface Coating Design for Dynamic Voltage Stability of Solid‐State Batteries

Abstract Intrinsic or interface thermodynamic voltage windows of solid electrolytes are often narrower than the operational voltage range needed by a full battery, thus various interface decomposition reactions can happen in a practical solid‐state battery. Experimentally, it is found that a proper battery design utilizing the reactions can lead to a dynamic evolution from interface instability to stability, giving the so‐called dynamic voltage stability for advanced battery performance. Here, first the state‐of‐the‐art understanding is articulated about how the dynamic voltage stability should be interpreted in physical picture and treated in computation, emphasizing the potential importance of nonequilibrium reaction pathways. The constrained ensemble computational approach is further applied across most types of solid‐state electrolytes to systematically evaluate and compare their dynamic stability voltage windows in response to the mechanical constriction effect. High‐throughput calculations are used to search for coating materials for different interfaces between sulfide, halide, and oxide electrolytes and typical cathode materials with enhanced dynamic voltage stability. A comparison with experiment is given to highlight the value of these computational predictions.

Wang, Yichao↗
DOE OSTI2018

Wrapping Nanocellulose Nets around Graphene Oxide Sheets

Constructing advanced functional nanomaterials with pre-designed organized morphologies from low-dimension synthetic and biological components is challenging. Herein, we report an efficient and universal amphiphilicity-driven assembly strategy to construct “hairy” flexible hybrid nanosheets with a 1D cellulose nanofibers (CNFs) net conformally wrapped around 2D graphene oxide (GO) monolayers. This interface-driven bio-synthetic assembly is facilitated by tailoring the surface chemistry of flexible GO sheets, resulting in individual sheets tightly surrounded by dense conformal nanocellulose network. The mechanical stability of the products far exceeds the compressive instability limits of both individual components. Finally, the CNF network significantly enhances the wetting ability of initial hydrophobic reduced GO nanosheets, allowing fast water transport combined with high filtration efficiency.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Application of machine learning interatomic potentials in heterogeneous catalysis

Heterogeneous catalysts are crucial in modern societies as they promote sustainability by enabling lower-energy pathways for various chemical reactions. While Density Functional Theory (DFT) computations can provide critical insights into how heterogeneous catalysts operate at the atomic level, they are limited by computational costs and unfavorable scaling with system size. Recently, machine learning interatomic potentials (MLIPs) have emerged as a promising alternative to DFT, offering near-DFT accuracy at significantly reduced cost. Here, in this perspective, we discuss the application of MLIPs in heterogeneous catalyst modeling as a surrogate for DFT. We detail how MLIPs have been applied in thermal catalysis to probe active sites, enable studying complex metallic and nanoporous catalysts, and investigate the reconstruction of catalytic surfaces. We review the use of MLIPs in electrocatalysis and photocatalysis, emphasizing their capabilities in studying transition metal oxide surfaces and solid–liquid interfaces. We also discuss the current limitations of MLIPs, particularly their challenges with transferability and description of non-local interactions. Finally, we conclude by identifying promising and underexplored domains in which MLIPs can further advance our understanding of heterogeneous catalysts.

Catalytic surfaces↗