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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 271 records · Page 15
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Control of polymorphism during epitaxial growth of hyperferroelectric candidate LiZnSb on GaSb (111)B

A major challenge for ferroelectric devices is the depolarization field, which competes with and often destroys long-range polar order in the limit of ultrathin films. Recent theoretical predictions suggest a new class of materials, termed hyperferroelectics, that should be robust against the depolarization field and enable ferroelectricity down to the monolayer limit. Here, the authors demonstrate the epitaxial growth of hexagonal LiZnSb, one of the hyperferroelectric candidate materials, by molecular-beam epitaxy on GaSb (111)B substrates. Due to the high volatility of all three atomic species, they find that LiZnSb can be grown in an adsorption-controlled window, using an excess zinc flux. Within this window, the desired polar hexagonal phase is stabilized with respect to a competing cubic polymorph, as revealed by x-ray diffraction and transmission electron microscopy measurements. First-principles calculations show that for moderate amounts of epitaxial strain and moderate concentrations of Li vacancies, the cubic LiZnSb phase is lower in formation energy than the hexagonal phase, but only by a few millielectronvolts per formula unit. Therefore, they suggest that kinetics plays a role in stabilizing the desired hexagonal phase at low temperatures. Their results provide a path toward experimentally demonstrating ferroelectricity and hyperferroelectricity in a new class of ternary intermetallic compounds.

42 ENGINEERING↗
DOE OSTI2021

Beryllium-driven structural evolution at the divertor surface

Erosion of the beryllium first wall material in tokamak reactors has been shown to result in transport and deposition on the tungsten divertor. Experimental studies of beryllium implantation in tungsten indicate that mixed W–Be intermetallic deposits can form, which have lower melting temperatures than tungsten and can trap tritium at higher rates. To better understand the formation and growth rate of these intermetallics, we performed cumulative molecular dynamics (MD) simulations of both high and low energy beryllium deposition in tungsten. In both cases, a W–Be mixed material layer (MML) emerged at the surface within several nanoseconds, either through energetic implantation or a thermally-activated exchange mechanism, respectively. While some ordering of the material into intermetallics occurred, fully ordered structures did not emerge from the deposition simulations. Targeted MD simulations of the MML to further study the rate of Be diffusion and intermetallic growth rates indicate that for both cases, the gradual re-structuring of the material into an ordered intermetallic layer is beyond accessible MD time scales(≤1 μs). However, the rapid formation of the MML within nanoseconds indicates that beryllium deposition can influence other plasma species interactions at the surface and begin to alter the tungsten material properties. Therefore, beryllium deposition on the divertor surface, even in small amounts, is likely to cause significant changes in plasma-surface interactions and will need to be considered in future studies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Spectroscopy of Palladium Nanoparticle Synthesis: Tailoring Nanoparticle Growth Parameters for Hydrogen Storage

Using palladium for hydrogen storage requires palladium (Pd) particles exhibiting specific parameters, including surface area, particle size, and particle shape, with increased interest in palladium nanoparticles (Pd NPs). In order to routinely monitor the synthesis of these particles a spectroscopic method is being developed using infrared (IR), Raman, and UV-Vis spectroscopy. By monitoring the production of Pd NPs, the growth of the NPs can be controlled to ensure quality of the product to match the desired finished particle specifications. For the reaction presented, the conversion of the intermediate tetraamminepalladium(II) chloride (PTC) to diamminepalladium(II) chloride (PDC) can influence the Pd NPs properties. This study is first being developed in lab bench scale quantities to allow ultimate control of the Pd NPs.

08 HYDROGEN↗
DOE OSTI2021

Sharp boundaries for the swampland

We reconsider the problem of bounding higher derivative couplings in consistent weakly coupled gravitational theories, starting from general assumptions about analyticity and Regge growth of the S-matrix. Higher derivative couplings are expected to be of order one in the units of the UV cutoff. Our approach justifies this expectation and allows to prove precise bounds on the order one coefficients. Our main tool are dispersive sum rules for the S-matrix. We overcome the difficulties presented by the graviton pole by measuring couplings at small impact parameter, rather than in the forward limit. We illustrate the method in theories containing a massless scalar coupled to gravity, and in theories with maximal supersymmetry.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Nano-imaging of strain-tuned stripe textures in a Mott crystal

The 4d transition metal perovskites Ca n+1 Ru n O 3n+1 have attracted interest for their strongly interacting electronic phases showing pronounced sensitivity to controllable stimuli like strain, temperature, and even electrical current. Through multi-messenger low-temperature nano-imaging, we reveal a spontaneous striped texture of coexisting insulating and metallic domains in single crystals of the bilayer ruthenate Ca 3 (Ti x Ru 1-x ) 2 O 7 across its first-order Mott transition at T ≈ 95K. We image on-demand anisotropic nucleation and growth of these domains under in situ applied uniaxial strain rationalized through control of a spontaneous Jahn-Teller distortion. Our scanning nano-susceptibility imaging resolves the detailed susceptibility of coexisting phases to strain and temperature at the transition threshold. Comparing these nano-imaging results to bulk-sensitive elastoresistance measurements, we uncover an emergent “domain susceptibility” sensitive to both the volumetric phase fractions and elasticity of the self-organized domain lattice. Our combined susceptibility probes afford nano-scale insights into strain-mediated control over the insulator-metal transition in 4d transition metal oxides.

36 MATERIALS SCIENCE↗
DOE OSTI2025

First indirectly driven liquid-DT filled double shell implosions at the National Ignition Facility

Double shell implosions aim to explore material mixing under fusion conditions in a volume burn geometry using high-Z metal pushers. High-Z pushers are more compressible than low-Z pushers enabling high stagnation pressure which reduces the required implosion speed while maintaining a low pusher adiabat despite strong shock heating. Additionally, the use of a small fuel mass reduces the fuel internal energy required for ignition, thus achieving stable platforms with reasonable fusion output to conduct controlled experiments. These factors make volume burn in a double shell implosion highly promising. Recently, a series of liquid-DT filled, indirectly driven, double shell implosions were conducted at the National Ignition Facility with laser drives reaching up to 1.5 MJ. These experiments achieved a maximum DT neutron yield of 1.67 × 10 14 (yield—479 J), DT ion temperature of 2.6 keV, fuel areal density (ρR) of 0.15 g/cm 2 , and stagnation pressure of 79 Gbar. Over the course of these shots, the DT neutron yield has increased by an order of magnitude largely from improved mitigation of outer shell assembly joint driven instability growth using thicker gold plating at the assembly joint. Further performance improvements are expected by enhancing outer-to-inner shell kinetic energy transfer and refined mitigation of degradations from engineering features such as the outer shell joint, fill tube, and surface roughness.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Supernova Hydrodynamics: A Lab-scale Study of the Blast-driven Instability Using High-speed Diagnostics

A novel experimental approach to study the blast-driven instability at a nondiffuse, gaseous interface with a density gradient is presented. Under Euler similarity, this approach enables study of dissipative-scale hydrodynamics relevant to many astrophysical and laboratory high energy density phenomena in a well-resolved manner. The instability is initiated by passing a Taylor–Sedov blast wave originating from a controlled detonation through a perturbed and stably stratified interface between two gases. The facility and driving blast wave are characterized to obtain repeatable conditions and capture large ensembles of time-resolved Mie scattering imaging that show consistent hydrodynamic development. We analyze the instability evolution between different gas pairs to demonstrate the wide range of development and turbulent behavior that may occur between different supernova layers. The mean evolution of the hydrodynamic instability is compared to a buoyancy–drag model that is frequently used to estimate perturbation growth in supernova mixing research. We propose a time delay to this model in order to reproduce the measured instability behavior and demonstrate model robustness in handling flows driven by a time-varying acceleration.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Understanding Time Dependence on Zinc Metal-Organic Framework Growth Using In Situ Liquid Secondary Ion Mass Spectrometry

The abundance of novel metal-organic framework (MOF) materials continues to increase as more applications are discovered for these highly porous, well-ordered crystalline adsorbents. The simplicity of its constituents allows for the design of new MOFs with virtue of functionality and pore topology towards target adsorbates. However, the fundamental understanding of how these frameworks age during nucleation and growth is mostly limited to speculation from simulation studies. In this effort, we utilize the microfluidic interface of liquid and vacuum in a unique SALVI device to analyze the formation and aging of the benchmark MOF-74 framework using time-of-flight secondary ion mass spectrometry (ToF-SIMS). Principal component analysis (PCA) of the SIMS mass spectra together with ex situ microscopy and porosimetry, provide new insights into the growth and aging process.

Sabale, Sandip R.↗
DOE OSTI2022

Design optimization for Richtmyer–Meshkov instability suppression at shock-compressed material interfaces

We report the Richtmyer–Meshkov instability (RMI) is a phenomenon that occurs at the interface of two substances of different densities due to an impulsive acceleration, such as a shock wave passing through this interface. Under these conditions, the instability can be seen as interface perturbations begin to grow into narrow jets or spikes of one substance that propagate into the other. In some cases, this interface may involve an elastic–plastic material, which can play a significant role in the development and behavior of the RMI. The ability to effectively control RMI jetting and spike growth is one major limiting factor in technological challenges, such as inertial confinement fusion, that involve using high-pressure shock waves to implode a fuel target. The propagation of RMI growth can lead to increased asymmetry in this implosion process and significantly reduce the obtained energy yield. We use hydrodynamics simulations of impactor shock-compression experiments and methods based in design optimization to suppress RMI spike growth by altering the geometry and other properties of a shock-compressed elastic–plastic material target that shares an interface with atmospheric air. These hydrodynamics simulations use an arbitrary Lagrangian–Eulerian method with a high-order finite element approach. Our results demonstrate that RMI suppression can be achieved by intentionally creating a separate upstream interface instability to counteract the growth of long narrow RMI spikes at an interface with initial perturbations.

36 MATERIALS SCIENCE↗
DOE OSTI2021

BiInO 3 phases under asymmetric in-plane strain

Density functional theory is used to study the effect of asymmetric in-plane strain on various BiInO 3 phases. Structural relaxation is carried out to simulate the growth of coherently strained epitaxial films on (001) oriented orthorhombic perovskite substrates. The results are in particular analyzed with respect to commercially available substrates in order to assess the stabilization of new and fundamentally interesting BiInO 3 phases. We find that a pyroxene-like Pcca phase is energetically more favorable than the bulk-like Pna2 1 structure on standard cubic substrate materials, such as SrTiO 3 . However, the presence of imaginary phonon modes suggests that this phase is dynamically instable. The bulk-like structure instead is stable over a wide range of lattice in-plane strain, but coherent growth requires substrates with unusually large lattice parameters. We suggest the use of lanthanate substrates in order to produce high-quality thin films of the bulk phase.

36 MATERIALS SCIENCE↗
DOE OSTI2022

CO2 Hydrogenation to Hydrocarbons over Fe/BZY Catalysts

This manuscript reports a CO2 hydrogenation process in a catalytic laboratory-scale packed-bed reactor using an Fe/BZY15 (BaZr0.8Y0.15O3-d) catalyst to form hydrocarbons (e.g., CH4, C2+) at elevated pressure of 30 bar and temperatures in the range 270 = T = 375 degrees C. The effects of temperature, feed composition (i.e., CO2/H2 ratio, and residence time (i.e., Weight Hourly Space Velocity (WHSV) are studied to understand the relationship between CO2 conversion and carbon selectivity. Catalyst characterization elucidates the relationships between the catalyst structure, surface adsorbates, and reaction pathways. Thermodynamic analyses guide the experimental conditions and assist interpreting results. While the feed composition and temperature influence the product distribution, the results suggest that the higher-carbon (C2+) selectivity and yield depend strongly on residence time. The results suggest that the CO2 hydrogenation reaction pathway is similar to Fischer-Tropsch (FT) synthesis. The reaction begins with CO2 activation to form CO, followed by chain-growth reactions similar to the FT process. The CO2 activation depends on the redox activity of the catalyst. However, the carbon chain growth depends primarily on the residence time. as is the case for the FT synthesis, high residence time (on the orders of hours) is required to achieve high C2+ yield. For such high residence times, catalyst-fouling carbon deposition can be problematic. The coke-resistant BZY15 catalyst support contributes to the catalytic activity and enables a coke-free operation for more than 100 h time-on-stream.

bi-functional catalyst↗
DOE OSTI2020

Development of lithium ion conducting interface between lithium metal and a lithium ion conducting ceramic using block polymers

The lithium-air (Li-air) technology developed by EDF uses an air electrode which works with an aqueous electrolyte, which prevent the use of unprotected lithium metal electrode. A Li+ ionic conductor glass ceramic is used to separate the aqueous electrolyte compartment from the negative lithium electrode. However, this glass-ceramic is not stable in contact with lithium, it is thus necessary to add a protective buffer layer. In another hand, this protection should ideally resist to lithium dendritic growth. It is in this context that this research project which has as goal the development of a protective buffer layer based on block copolymer electrolytes (BCE) between the lithium metal and the lithium ionic conductor ceramic, for lithium-air battery. In a first part, the BCE is studied in lithium-lithium symmetric cells, in order to determine their electrochemical properties such as ionic conductivity, steady state transference number, and finally their resistance to dendritic growth during cycling. Several characterization techniques were employed and especially hard X-ray micro-tomography to analyze the lithium morphology before and after cycling. For single-ion BCE, we expect to suppress dendritic growth, however, we report here for the first time, the visualization of a homogeneous growth of lithium but the formation of dense lithium objects. In another part, the composite BCE-ceramic is studied by electrochemical impedance spectroscopy (EIS). The cycling of lithium-composite-lithium symmetric cells and the analysis of the EIS measurement after each cycle permit to determine if the dendrites have cross the protective layer and are in contact with the ceramic. Besides, the quantification of the polarization loss at the interface polymer-ceramic is evaluated by polarization experiments. This contribution is found to be small.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Atomic Layer Deposition Niobium Nitride Films for High-Q Resonators

Niobium nitride (NbN) is a useful material for fabricating detectors because of its high critical temperature and relatively high kinetic inductance. In particular, NbN can be used to fabricate nanowire detectors and mm-wave transmission lines. When deposited, NbN is usually sputtered, leaving room for concern about uniformity at small thicknesses. In this work, we present atomic layer deposition niobium nitride (ALD NbN) as an alternative technique that allows for precision control of deposition parameters such as film thickness, stage temperature, and nitrogen composition. Atomic-scale control over film thickness admits a high degree of uniformity for films 4–30 nm thick; control over deposition temperature gives rise to growth rate changes, which can be used to optimize film thickness and critical temperature. In order to charac- terize ALD NbN in the radio-frequency regime, we construct single-layer micro- wave resonators and test their performance as a function of stage temperature and input power. ALD processes can admit high resonator quality factors, with ≥ 43% of resonators above Q i = 10 6 , which in turn increase detector multiplexing capabilities. i Furthermore, we find critical temperatures in the range of 7.5–10.9 K that vary as a function of cycle count and deposition temperature.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Strongly Anisotropic Thermomechanical Response to Shock Wave Loading in Oriented Samples of the Triclinic Molecular Crystal 1,3,5-Triamino-2,4,6-trinitrobenzene

All-atom molecular dynamics (MD) simulations were used to study shock wave loading in oriented single crystals of the highly anisotropic triclinic molecular crystal 1,3,5-triamino-2,4,6-trinitrobenzene (TATB). The crystal structure consists of planar hydrogen-bonded sheets of individually planar TATB molecules that stack into graphitic-like layers. Shocks were studied for seven systematically prepared crystal orientations with limiting cases that correspond to shock propagation exactly perpendicular and exactly parallel to the graphitic-like layers. The simulations were performed for initially defect-free crystals using a reverse-ballistic configuration that generates explicit, supported shocks. Final longitudinal stress components are between ≈8.5 and ≈10.5 GPa for the 1.0 km s –1 impact speed studied. Orientation-dependent properties are reported including shock speeds, stresses, temperatures, compression ratios, and local material strain rates. Spatiotemporal maps of the temperature, stress tensor, material flow, and molecular orientations reveal complicated processes that arise for specific shock directions. Furthermore, the results indicate that TATB shock response is highly sensitive to crystal orientation, with significant qualitative differences for the time evolution of the stress tensor and temperature, elastic/inelastic compression response, defect formation and growth, critical von Mises stress, and strain rates during shock rise that span nearly an order of magnitude. A variety of inelastic deformation mechanisms are identified, ranging from crumpling of graphitic-like layers to dislocation-mediated plasticity to intense shear strain localization. To our knowledge, these are the first systematic MD simulations and analysis of explicit shock wave propagation along nontrivial crystal directions in a triclinic molecular crystal.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Localization dynamics in a centrally coupled system

In systems in which interactions couple a central degree of freedom and a bath, one would expect signatures of the bath's phase to be reflected in the dynamics of the central degree of freedom. This has been recently explored in connection with many-body localized baths coupled with a central qubit or a single-cavity mode - systems with growing experimental relevance in various platforms. Such models also have an interesting connection with Floquet many-body localization via quantizing the external drive, although this has been relatively unexplored. Here we adapt the multilayer multiconfigurational time-dependent Hartree (ML-MCTDH) method, a well-known tree tensor network algorithm, to numerically simulate the dynamics of a central degree of freedom, represented by a d-level system (qudit), coupled to a disordered interacting one-dimensional spin bath. ML-MCTDH allows us to reach ≈10 2 lattice sites, a far larger system size than what is feasible with exact diagonalization or kernel polynomial methods. From the intermediate time dynamics, we find a well-defined thermodynamic limit for the qudit dynamics upon appropriate rescaling of the system-bath coupling. The spin system shows similar scaling collapse in the Edward-Anderson spin-glass order parameter or entanglement entropy at relatively short times. At longer timescales, we see slow growth of the entanglement, which may arise from dephasing mechanisms in the localized system or long-range interactions mediated by the central degree of freedom. Similar signs of localization are shown to appear as well with unscaled system-bath coupling.

1-dimensional spin chains↗
DOE OSTI2024

Anisotropic magnetism of polymorphic ErAl 3

ErAl 3 can form in either a trigonal (α) or cubic (β) polymorph and this paper investigates the physical properties of these polymorphs through characterizations of single crystals grown in an aluminum flux. Here, we demonstrate that polymorph selection can be achieved based on the nominal composition of the crystal growth. Magnetic measurements confirm that both β-ErAl 3 and α-ErAl 3 order antiferromagnetically at low temperatures. β-ErAl 3 undergoes antiferromagnetic ordering at a Néel temperature T N = 5.1 K, and the transition is suppressed continually with applied field. α-ErAl 3 displays more complex behavior, with successive magnetic transitions at T N = 5.7 K and T 2 = 4.6 K for zero field, where heat capacity and dilatometry measurements evidence that these transitions are second and first order, respectively. Under magnetic field, strong anisotropy is revealed in α-ErAl 3 , with several steplike metamagnetic transitions observed below T 2 for H ∥ c. These transitions produce sequential magnetization plateaus near one-half of the apparent saturation magnetization. The electrical resistivity of α-ErAl 3 is strongly coupled to its magnetism. At T = 2 K, we observe a positive magnetoresistance reaching 60%, with distinct anomalies at the metamagnetic transitions. The results are summarized in H-T phase diagrams that demonstrate complex magnetic behavior for α-ErAl 3 , suggesting an important role of competing interactions in this metallic system that possesses characteristics of Ising physics.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Epitaxial growth of rock salt MgZrN 2 semiconductors on MgO and GaN

Ternary nitride compound semiconductors have attracted recent attention as electronic materials since their properties can be tuned by cation stoichiometry and ordering. A recently discovered example is MgZrN 2 , a ternary analog to the rock salt semiconductor ScN. MgZrN 2 has a larger bandgap and stronger dielectric response than the binary compound. Polycrystalline thin films of MgZrN 2 have been studied, but demonstration of high-quality growth is still required to establish its suitability for technological applications. Here, we report on epitaxial growth of MgZrN 2 thin films on (100) and (111) MgO substrates and (001) GaN templates. The MgZrN 2 composition is confirmed by Rutherford backscattering spectrometry, showing no oxygen in the film except for a thin surface oxide layer. Epitaxial growth results in MgZrN 2 with x-ray diffraction rocking curves with a full-width at half-maximum in the range of 0.3–3.0°, depending on the substrate. Transmission electron microscopy analysis of the MgZrN 2 film grown on a (111) MgO substrate confirms epitaxial growth and shows a sharp film/substrate interface. In-plane temperature-dependent Hall effect measurements show that the material is an n-type semiconductor with a relatively high concentration ( n 300K ≈ 10 19 –10 20 cm -3 ) of thermally activated electrons. Room-temperature transport measurements show a conductivity of 25 S cm -1 and a Seebeck coefficient of -80 μ V K -1 . Overall, these results provide an important step toward integration of rock salt MgZrN 2 with other technological nitrides for device applications.

36 MATERIALS SCIENCE↗
DOE OSTI2020

A Model of Grain Boundary Complexion Transitions and Grain Growth in Yttria-Doped Alumina

In this work, we present a physically-parameterized microstructure evolution model for the Yttria-doped alumina system. Yttria-doped alumina is a well-known ceramic system which undergoes first-order phase-like transitions at grain boundaries, which can radically alter interface properties. The change in interfacial properties in turn can radically change microstructure outcomes during processing, including the induction of abnormal grain growth modes. In this work, we develop a simulation that evolves alumina microstructure as a function of yttria concentration and temperature. In the window studied, we achieve strong agreement with reviewed experimental results in identifying the windows for large grains, small grains, abnormal grain growth, and complexion transition kinetics. We then apply the model to study and demonstrate how the possible inclusion of second-phase particles or uneven solute distribution profiles will impact microstructure evolution. It is found that particles do not significantly affect abnormal grain growth in the window studied (but do lead to reduced grain size through pinning effects). It is found that even modest amounts of solute inhomogeneity will result in substantial changes in microstructure outcomes, frequently leading to clusters of abnormal grains. This model largely corroborates the expectations and hypotheses made from recent experimental studies in oxide-doped alumina systems. Further, it is found that there exists a peak transition fraction for the system at which abnormal grain size tends to be maximized.

Grain Growth, Grain Boundary Complexion, abnormal ↗