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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 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Effects of catalyst droplets on wire growth and the resulting branched structures during VLS growth

Vapor-liquid-solid (VLS) method is vastly employed to grow hierarchical structures with unique properties. However, key questions remain, such as what controls the branched structures and what the roles of catalyst droplet size are during the growth. Here, an in-depth understanding of the kinetics of the nucleation, growth, and subsequent coalescence processes of Bi liquid catalyst droplets is provided by direct observation of PbSe branched wire growth in an environmental transmission electron microscope. This brings a kinetic control of the branch density by varying the parameters, such as temperature. In addition, the dependence of wire growth rate on the catalyst droplet size is revealed, i.e., the smaller the catalyst size the larger the wire growth rate, unlike the wire growth controlled by Gibbs-Thomson effect, possibly due to different mass transport pathways and atomic surface diffusion. These results extend the fundamental understanding of the VLS growth mechanism of branched structures and benefit the structure design of hierarchical materials with tailored properties.

36 MATERIALS SCIENCE↗
DOE OSTI2024

A Personal Journey in Nanoscience via Developing and Applying Liquid Phase TEM

Liquid phase TEM has attracted widespread attention in recent years as a groundbreaking tool to address various fundamental problems in nanoscience. It has provided the opportunity to reveal many unseen dynamic phenomena of nanoscale materials in solution processes by direct imaging through liquids with high spatial and temporal resolution. After my earlier work on real-time imaging of the nucleation, growth, and dynamic motion of nanoparticles in liquids by developing high-resolution liquid phase transmission electron microscopy (TEM) down to the sub-nanometer level, I established my own research group at Lawrence Berkeley National Lab in 2010. My group focuses on developing and applying liquid phase TEM to investigate complex systems and reactions. We have studied a set of scientific problems centered on understanding how atomic level heterogeneity and fluctuations at solid-liquid interfaces impact nanoscale materials transformations using advanced liquid phase TEM. This article describes my personal journey in nanoscience, highlighting the main discoveries of my research group using liquid phase TEM as a unique tool. Some perspectives on the impacts of liquid phase TEM and the future opportunities in nanoscience and nanotechnology enabled by liquid phase TEM are also included.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Dislocation nano-hydrides in nickel: Nucleation, evolution and effects on dislocation behaviors

Nano-hydrides have been predicted to precipitate at the core of edge dislocations in the Ni-H system, a mechanism that may promote hydrogen embrittlement. However, nano-hydride nucleation, growth, and effects on dislocation behavior have seldom been explored. This work combines molecular dynamics grand canonical Monte Carlo (MD-GCMC) simulations and continuum modeling to uncover a wide range of phenomena linked to dislocation nano-hydrides. Simulations reveal that nano-hydrides can be stabilized at dislocation cores with all character angles, including screw segments, due to the hydrostatic stresses around the cores of the Shockley partials. Nano-hydride nucleation takes place in these regions, and growth is dictated by the character angle θ of the perfect dislocation. The equilibrium stacking fault width d eq varies dynamically to increase the local hydrostatic stress field and facilitate the formation of the nano-hydride, forming a constriction-like feature and leading to three distinct behaviors: d eq decreases for θ > 30°, d eq remains unchanged for θ = 30°, and d eq increases for θ < 30°. Remote hydrostatic and Escaig stresses are also shown to influence the nucleation stage, implying stress concentrations such as those ahead of crack tips may facilitate nano-hydride precipitation. Moreover, we identify a new hydrogen-induced 60° dislocation reaction that emits a Shockley partial on a conjugate plane, with potential implications for twin nucleation. Testable predictions from this study are then used to reinterpret previous results from the literature. In conclusion, these findings provide a comprehensive framework to assess nano-hydride formation and evolution at dislocations in nickel and other face-centered cubic metals, with important implications to hydrogen embrittlement.

Dislocations↗
DOE OSTI2020

Exascale-capable cellular automaton for nucleation and grain growth

This model is a cellular automata-based algorithm used to predict grain-scale microstructure development. Nucleation and growth of existing grains are considered in an initially liquid domain, where the temperature field evolution is either driven through heat transport simulation data or a frozen temperature approximation (i.e., a constant cooling rate and a fixed thermal gradient). The growth of grains is based on the decentered octahedron algorithm published by Gandin and Rappaz (https://doi.org/10.1016/S1359-6454(96)00303-5), where the grain envelopes are tracked as approximations of the evolving dendritic growth front. The input heat transport data, which can come from simulation of an arbitrary processing technique, consists of coordinates and times at which said coordinates fall below the liquidus and solidus temperatures for the final time. As a result, only the final solidification of a given region is modeled (no remelting). The code is designed to be compatible with pre-Exascale architectures, and uses MPI and the Kokkos library to decompose the computational domain and offload solidification calculations to GPUs.

Rolchigo, MatthewR.↗
DOE OSTI2026

Predicting critical heat flux using localized sensing at invisible vapor-liquid interfaces

Predicting critical heat flux (CHF) in two-phase electronics cooling systems remains a significant challenge due to the sudden onset of boiling crisis and the difficulty in directly visualizing vapor-liquid interfaces. Existing sensing methods rely on lagging temperature measurements, optically accessible systems, or spatially averaged signals that cannot pinpoint CHF initiation at localized high-heat-flux regions. Here, we report a planar capacitive sensing approach that enables real-time, localized detection of vapor-liquid interface dynamics for CHF prediction in boiling heat transfer. The capacitive sensor exploits the dielectric constant difference between liquid and vapor phases to capture bubble nucleation, growth, and departure dynamics with a temporal resolution down to 2 ms. The capacitive sensing reveals distinct signals across boiling regimes: from high-frequency fluctuations during strong nucleate boiling to low-frequency fluctuations with increased amplitudes when approaching CHF. The multi-sensor array experiments demonstrate real-time localized sensing, where each sensor responds exclusively to boiling in its immediate vicinity without crosstalk from neighboring regions. This non-intrusive sensing approach provides predictive rather than lagging sensing signals of CHF occurrence, offering predictive diagnosis of two-phase liquid cooling for the thermal management of high-power-density electronics.

CHF↗
DOE OSTI2021

The mobility of small, over-pressurized helium bubbles in tungsten at 2000 K

Fusion reactor environments inevitably lead to the formation of high-pressure helium bubbles whose nucleation, growth, and diffusion strongly impact the performance of plasma-facing components. Here this research describes a diffusion mechanism of over-pressurized bubbles via a sequence of Frenkel pair nucleation, self-interstitial migration, and Frenkel pair annihilation. Molecular dynamics was used to simulate the diffusion of small bubbles in tungsten at 2000 K with helium-per-vacancy ratios in the range of 4.5 to 7. The diffusion coefficients are calculated and their dependence on helium content, number of vacancies, and number of attached self-interstitials is characterized. It is found that bubbles are most mobile when the nucleation/annihilation rates of Frenkel pairs are nearly equal and when the bubbles nucleate and annihilate a single self-interstitial. All bubbles experience a peak diffusivity, which can be as high as 10 -11 m 2 /s decreasing with bubble size. The calculated diffusion coefficients provide valuable insight into the mobility of small, high-pressure bubbles, and can be used as input parameters in mesoscale models to improve predictions of plasma-surface interactions. (LA-UR-21-21881)

36 MATERIALS SCIENCE↗
DOE OSTI2022

Phase transformation and growth mechanism of RF sputtered ferroelectric lead scandium tantalate (PbSc 0.5 Ta 0.5 O 3 ) films

Lead scandium tantalate (PbSc 0.5 Ta 0.5 O 3 , PST), an order/disorder ferroelectric, is a potential candidate for electrocaloric cooling and pyroelectric infrared (IR) detector. In this work, we report the phase transformation kinetics from two series of samples containing pure amorphous and mixture of amorphous and pyrochlore to desired perovskite phase using postdeposition rapid thermal processing (RTP) as well as growth mechanism of RF sputtered PST thin films using excess lead target on platinized silicon (Pt/Ti/SiO 2 /Si) substrates. We find that small changes in the temperature ramp have a large effect on the degree of perovskite conversion (ferroelectric phase), orientation (crystallographic texture), and long-range order parameter (< S 111 >). Through isothermal annealing, we obtained optimal perovskite phase at ≥700°C temperature. The phase transformation is characterized by spontaneous formation of center-type in-plane radial rosette-like structures revealed by scanning electron microscopy. The PST perovskite crystallites were found to coexist with pyrochlore in RTP annealed films. The volume fractions for perovskite and pyrochlore phase were obtained from the analysis of “rosettes” and respective X-ray diffraction intensities which helped to determine various parameters associated with phase kinetics (n, k, and activation energy, Ea) and accompanying growth. The effective activation energies of perovskite transition and growth were found to be 332 ± 11 kJ/mol (345 ± 11 kJ/mol) and 114 ± 10 kJ/mol (122 ± 10 kJ/mol), respectively, for pure amorphous only (and mixed amorphous and pyrochlore) phase following nucleation-growth controlled Avrami's equation. A linear growth rate (n~1) for the perovskite phase indicates predominant interface-controlled process and diffusion-limited phenomena thus inhibiting rosette size owing to reactant depletion and soft impingement at the grain boundary. However, the growth behavior is isotropic in two-dimension parallel to the plane of the substrates for both sample series. Furthermore, lead loss was severe for in-situ growth and RTP combined with conventional furnace annealing than those of RTP only films, which were closer to stoichiometric albeit with excess lead and marginal oxygen vacancies (V o ).

36 MATERIALS SCIENCE↗
DOE OSTI2021

Unraveling compacted graphite evolution during solidification of cast iron using in-situ synchrotron X-ray tomography

In spite of many years of research, the physical phenomena leading to the evolution of compacted graphite (CG) during solidification is still not fully understood. In particular, it is unknown how highly branched CG aggregates form and evolve in the semi-solid, and how local microstructural variations at micrometer length scale affect this growth process. We present here the first time-resolved synchrotron tomography combined with a bespoke high-temperature environmental cell that allows direct observation of the evolution of CG and relates this dynamic process to the local surrounding microstructures in a cast iron sample during repeated melting and solidification. Distinct processes are identified for the formation of CG involving the nucleation, growth, development of branches and interconnection of graphite particles, ultimately evolving into highly branched graphite aggregates with large sizes and low sphericities. CG is found to nucleate with a spheroidal or a plate-like shape, developing branches induced by high carbon concentration, e.g. thin melt channels. Additionally, CG grows much faster than spheroidal graphite during subsequent cooling in solid state. The direct visualization of the dynamic solidification process provides unprecedented new insights into formation mechanisms of CG and correlating factors such as local microstructural variations, and guides the development of CG iron solidification models.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Robustness of Optical Response for Self-Assembled Plasmonic Metamaterials with Morphological Disorder and Surface Roughness

Bottom-up fabrication of metallized biotemplated nanostructures to form specific plasmonic nanoresonators holds promise as a means of achieving large-scale optical metamaterials. However, in contrast to top-down methods, the stochastic growth of self-assembled nanoresonators is prone to significant disorder and surface roughness, which naturally raise an important question about the robustness of their resonant properties in terms of structural imperfections. An aggregated-random-sphere model is developed to mimic the nucleated growth of metallized DNA origami assembly, leading to meta-atoms with realistic, experimentally observed morphological disorder and surface roughness. Using the well-known split-ring-resonator (SRR) motif as an example, the resonant properties of meta-atoms under different levels of roughness are investigated and a strong tolerance of optical response against morphological disorder is revealed. It is found that in SRRs, even with dramatic roughness introduced, the expected resonances are still observed, despite broadening line shapes compared to ideal smooth structure. Only for extreme disorder, which causes drastic segmentation of SRRs, does the resonant response disappear. Finally, the demonstrations are very encouraging for the prospects of bottom-up fabrication toward versatile functional metamaterials and metadevices.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Kinetics of Carbon Condensation in Detonation of High Explosives: First-Order Phase Transition Theory Perspective

We report the kinetics of carbon condensation, or carbon clustering, in detonation of carbon-rich high explosives is modeled by solving a system of rate equations for concentrations of carbon particles. Unlike previous efforts, the rate equations account not only for the aggregation of particles but also for their fragmentation in a thermodynamically consistent manner. Numerical simulations are performed, yielding the distribution of particle concentrations as a function of time. In addition to that, analytical expressions are obtained for all the distinct steps and regimes of the condensation kinetics, which facilitates the analysis of the numerical results and allows one to study the sensitivity of the kinetic behavior to the variation of system parameters. The latter is important because the numerical values of many parameters are not reliably known at present. The theory of the kinetics of first-order phase transitions is found adequate to describe the general kinetic trends of carbon condensation, as described by the rate equations. Such physical phenomena and processes as the coagulation, nucleation, growth, and Ostwald ripening are observed, and their dependence on various system parameters is studied and reported. It is believed that the present work will become useful when analyzing the present and future results for the kinetics of carbon condensation, obtained from experiments or atomistic simulations.

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

Pressure-tailored lithium deposition and dissolution in lithium metal batteries

Unregulated lithium (Li) growth is the major cause of low Coulombic efficiency, short cycle life and safety hazards for rechargeable Li metal batteries. Strategies that aim to achieve large granular Li deposits have been extensively explored, and yet it remains a challenge to achieve the ideal Li deposits, which consist of large Li particles that are seamlessly packed on the electrode and can be reversibly deposited and stripped. In this work, we report a dense Li deposition (99.49% electrode density) with an ideal columnar structure that is achieved by controlling the uniaxial stack pressure during battery operation. Using multiscale characterization and simulation, we elucidate the critical role of stack pressure on Li nucleation, growth and dissolution processes and propose a Li-reservoir-testing protocol to maintain the ideal Li morphology during extended cycling. The precise manipulation of Li deposition and dissolution is a critical step to enable fast charging and a low-temperature operation for Li metal batteries.

25 ENERGY STORAGE↗
DOE OSTI2025

Isolated vesicles in submarine pumice: insights from the 2019 Volcano F eruption, Kingdom of Tonga

No reliable method can distinguish between subaerial and submarine pumice, but recent work shows that highly vesicular (total porosity, φ > 65%) submarine pumice from the 2012 Havre and 2021 Fukutoku Oka-no-Ba eruptions contains abundant isolated porosity (connectivity, C < 0.6). This differs from textural measurements of subaerial pumice with similarly high vesicularities, where high connectivities (C > 0.8) are often measured. To investigate the implications of this under-studied texture for bubble nucleation, growth, and coalescence dynamics at submarine eruptions, we analyze the textural characteristics of rafted pumice clasts from the 2019 submarine eruption of Volcano F, located along the Tonga-Kermadec Arc. We examined clasts collected while floating near the vent (50–200 km) and distally on the shores of Fiji (900 km). Using helium pycnometry and X-ray tomography (XRT), we quantified porosity and connectivity in 45 pumice lapilli, classifying them by vesicle macrotexture and edge morphology. Microvesicular clasts, the majority of which have breadcrust and cauliflower textures, exhibit the lowest connectivities (C = 0.61 ± 0.2), while macrovesicular clasts have high connectivities with C ~ 1. We propose that isolated porosity abundance varies according to clast location in the eruption column post-fragmentation. Microvesicular clasts erupted on the edges of the column and experienced high levels of seawater ingestion and subsequent quenching of the entire clast. Macrovesicular clasts, in contrast, erupted in the center of the eruption column and were thus thermally insulated, allowing magmatic bubbles in the molten pumice to nucleate, grow, and coalesce for longer. Our results and interpretation imply that low connectivity, microvesicular clasts preserve pre and syn-eruptive bubble processes at the 2019 Volcano F eruption.

Permeability↗
DOE OSTI2026

Towards the Ultimate Strength of Medium‐Entropy Alloys Through Pulsed Lasers

The tensile strength of metals at extreme strain rates is a key predictor of their performance in ballistic and structural impact applications. An important experimental method to reach these extreme strain rates is the use of high-amplitude, short-duration pulsed lasers. The Jupiter Laser Facility at the Lawrence Livermore National Laboratory enabled probing for the first time the mechanical response of several promising High Entropy Alloys at times on the order of nanoseconds (strain rates of ∼10 7 and ∼10 9 s −1 ). The measured strength is in the range of 6 to 10 GPa, ten times the quasistatic value. The mechanisms of plastic deformation and failure were identified and quantified through analysis and molecular dynamics simulation. The reflected wave amplitudes, obtained by VISAR, were used to determine the tensile (spall) stress. The high tensile strength obtained is due to two factors: the strain-rate dependence of plastic flow and the kinetics of void nucleation, growth, and coalescence. The experimental results are compared with an analytical prediction considering both grain-interior and grain-boundary void initiation. Molecular dynamics simulations, conducted at strain rates of 10 8 and 10 9 s −1 , rationalize the experimental results. In conclusion, they provide valuable information about the process of failure evolution, and reveal that grain boundary separation plays a pivotal role in spalling.

Materials science↗
DOE OSTI2022

Stable Anode–Free All–Solid–State Lithium Battery through Tuned Metal Wetting on the Copper Current Collector

A stable anode-free all-solid-state battery (AF-ASSB) with sulfide-based solid-electrolyte (SE) (argyrodite Li 6 PS 5 Cl) is achieved by tuning wetting of lithium metal on “empty” copper current-collector. Lithiophilic 1 µm Li 2 Te is synthesized by exposing the collector to tellurium vapor, followed by in situ Li activation during the first charge. The Li 2 Te significantly reduces the electrodeposition/electrodissolution overpotentials and improves Coulombic efficiency (CE). During continuous electrodeposition experiments using half-cells (1 mA cm –2 ), the accumulated thickness of electrodeposited Li on Li 2 Te–Cu is more than 70 µm, which is the thickness of the Li foil counter-electrode. Full AF-ASSB with NMC811 cathode delivers an initial CE of 83% at 0.2C, with a cycling CE above 99%. Additionally, cryogenic focused ion beam (Cryo-FIB) sectioning demonstrates uniform electrodeposited metal microstructure, with no signs of voids or dendrites at the collector-SE interface. Electrodissolution is uniform and complete, with Li 2 Te remaining structurally stable and adherent. By contrast, an unmodified Cu current-collector promotes inhomogeneous Li electrodeposition/electrodissolution, electrochemically inactive “dead metal,” dendrites that extend into SE, and thick non-uniform solid electrolyte interphase (SEI) interspersed with pores. Density functional theory (DFT) and mesoscale calculations provide complementary insight regarding nucleation-growth behavior. Unlike conventional liquid-electrolyte metal batteries, the role of current collector/support lithiophilicity has not been explored for emerging AF-ASSBs.

36 MATERIALS SCIENCE↗
DOE OSTI2023

ATRP Enhances Structural Correlations In Polymerization–Induced Phase Separation**

Synthetic methods to control the structure of materials at sub–micron scales are typically based on the self–assembly of structural building blocks with precise size and morphology. On the other hand, many living systems can generate structure across a broad range of length scales in one step directly from macromolecules, using phase separation. Here, we introduce and control structure at the nano– and microscales through polymerization in the solid state, which has the unusual capability of both triggering and arresting phase separation. In particular, we show that atom transfer radical polymerization (ATRP) enables control of nucleation, growth, and stabilization of phase–separated poly–methylmethacrylate (PMMA) domains in a solid polystyrene (PS) matrix. ATRP yields durable nanostructures with low size dispersity and high degrees of structural correlations. Furthermore, we demonstrate that the length scale of these materials is controlled by the synthesis parameters.

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

The Application of Differential Scanning Calorimetry to Investigate Precipitation Behavior in Nickel-Base Superalloys Under Continuous Cooling and Heating Conditions

In this study, a suite of experimental tools and fast-acting, numerical-simulation techniques was used to quantify the precipitation behavior of three nickel-base superalloys: IN-100, LSHR, and 718. Experimental methods comprised differential scanning calorimetry (DSC) to establish the specific heat as a function of temperature and selected direct-resistance heating trials (using a Gleeble ® machine) to obtain samples for microstructural analysis. For the DSC experiments, each alloy was cooled at a prescribed constant rate (between 5 and 20 K/min) after an initial soak/equilibration in the high-temperature, single-phase (supersolvus) temperature regime. On-heating DSC trials beginning at ambient temperature were also performed on alloy 718 in three different starting conditions: super- δ -solvus solution treated and water quenched (denoted as ST), solution treated and aged (STA), and solution treated and overaged (STOA). DSC results, revealing the thermal signatures associated with the kinetics of precipitation of γ ' (IN-100, LSHR) or γ ' and γ " (718), were interpreted using a previously-developed fast-acting routine that treats concurrent nucleation, growth, coarsening, and dissolution. For these simulations, special attention was paid to various thermo-kinetic input parameters including equilibrium solvus-approach curves, bulk free energies of transformation, matrix-precipitate interface energies, and effective diffusivities. For the γ - γ ' superalloys (IN-100 and LSHR), estimates of precipitate volume fraction as a function of temperature from the specific-heat data revealed semi-quantitative agreement with simulation predictions. For the γ - γ '- γ " superalloy (718), simulation predictions of precipitate volume fractions were converted to specific heat as a function of temperature and showed semi-quantitative agreement with the direct measurements.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Anomaly Detection in Materials Digital Twins with Multiscale ICME for Additive Manufacturing

Detecting anomaly in fatigue and fracture experimental materials science is an interesting yet challenging topic. The reasons are threefold. First, the anomalous microstructure feature that gives rise to structural failure is small, sometimes in the order of 10 -7 of the interrogated volume. This, in turn, results in a highly imbalanced classification problem in machine learning (ML). Second, the consequence is high, in the sense that the test specimen is destructed in such case. Third, the convolution between microstructure stochasticity and the small probability of void nucleation, growth, and coalescence makes failure and fracture a hard-to-predict and challenging problem in materials science due to its irreproducibility, even experimentally. In this paper, we developed a materials digital twin and applied anomaly detection methods to detect voids and anomaly in additive manufacturing (AM). The materials digital twin is driven by two integrated computational materials engineering (ICME) models, which are kinetic Monte Carlo (kMC) and crystal plasticity finite element method (CPFEM). In conclusion, we demonstrated that by using anomaly detection, it is possible to detect voids and other defects in materials digital twin, which paves way for future research in integrating materials digital twin with its physical counterpart.

ICME↗
DOE OSTI2024

Atomistic evidence of nucleation mechanism for the direct graphite-to-diamond transformation

The direct graphite-to-diamond transformation mechanism has been a subject of intense study and remains debated concerning the initial stages of the conversion, the intermediate phases, and their transformation pathways. Here, we successfully recover samples at the early conversion stage by tuning high-pressure/high-temperature conditions and reveal direct evidence supporting the nucleation-growth mechanism. Atomistic observations show that intermediate orthorhombic graphite phase mediates the growth of diamond nuclei. Furthermore, we observe that quenchable orthorhombic and rhombohedra graphite are stabilized in buckled graphite at lower temperatures. These intermediate phases are further converted into hexagonal and cubic diamond at higher temperatures following energetically favorable pathways in the order: graphite → orthorhombic graphite → hexagonal diamond, graphite → orthorhombic graphite → cubic diamond, graphite → rhombohedra graphite → cubic diamond. Furthermore, these results significantly improve our understanding of the transformation mechanism, enabling the synthesis of different high-quality forms of diamond from graphite.

Graphite-diamond phase transformation↗