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At least 1,135 records · Page 63
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Understanding Microstructure Variability in Vapor-Deposited Energetic Materials by Using Phase-Field Methods

Critical components, such as detonators, in Sandia's stockpile contain heterogeneous materials whose performance and reliability depend on accurate, predictive models of coupled, complex phenomena to predict their synthesis, processing, and operation. Ongoing research in energetic materials has shown that microstructural properties, such as density, pore-size, morphology, and specific surface area are correlated to their initiation threshold and detonation behavior. However, experiments to study these specific characteristics of energetic materials are challenging and time consuming. Therefore, in this work, we turn to mesoscale modeling methods that may be capable of reproducing some observed phenomena to refine and predict outcomes beforehand. Even so, we have no physics-based modeling capability to predict how the microstructure of an energetic material will evolve over near- and long-term time scales. Thus, the goal of this work is to (i) identify any knowledge gaps in how the underlying microstructure forms and evolves during the synthesis process, and (ii) develop and test a mesoscale phase-field model for vapor deposition to capture critical mechanisms of microstructure formation, evolution, and variability in vapor-deposited energetic materials, such as processing conditions, material properties, and substrate interactions. Based on this work, the phase-field method is shown to be a valuable tool for developing the necessary models containing coupled, complex phenomena to investigate and understand the synthesis and processing of energetic materials.

36 MATERIALS SCIENCE↗
DOE OSTI2021

A duality-based coupling of Cosserat crystal plasticity and phase field theories for modeling grain refinement

High-rate deformation processes of metals entail intense grain refinement and special attention needs to be paid to capture the evolution of microstructure. In this article, a new formulation for coupling Cosserat crystal plasticity and phase field is developed. A common approach is to penalize kinematic incompatibility between lattice orientation and displacement-based elastic rotation. However, this can lead to significant solution sensitivity to the penalty parameter, resulting in low accuracy and convergence rates. To address these issues, a duality-based formulation is developed which directly imposes the rotational kinematic compatibility. A weak inf-sup-based skew-symmetric stress projection is introduced to suppress instabilities present in the dual formulation. An additional least squares stabilization is introduced to suppress the spurious lattice rotation with a suitable parameter range derived analytically and validated numerically. The required high-order continuity is attained by the reproducing kernel approximation. It is observed that equal order displacement-rotation-phase field approximations are stable, which allows efficient employment of the same set of shape functions for all independent variables. The proposed formulation is shown to yield superior accuracy and convergence with marginal parameter sensitivity compared to the penalty-based approach and successfully captures the dominant rotational recrystallization mechanism including block dislocation structures and grain boundary migration.

42 ENGINEERING↗
DOE OSTI2022

Miscibility of rock and ice in the interiors of water worlds

Abstract Super-Earths and sub-Neptunes are the most common planet types in our galaxy. A subset of these planets is predicted to be water worlds, bodies that are rich in water and poor in hydrogen gas. The interior structures of water worlds have been assumed to consist of water surrounding a rocky mantle and iron core. In small planets, water and rock form distinct layers with limited incorporation of water into silicate phases, but these materials may interact differently during the growth and evolution of water worlds due to greater interior pressures and temperatures. Here, we use density functional molecular dynamics (DFT-MD) simulations to study the miscibility and interactions of enstatite (MgSiO 3 ), a major end-member silicate phase, and water (H 2 O) at extreme conditions in water world interiors. We explore pressures ranging from 30 to 120 GPa and temperatures from 500 to 8000 K. Our results demonstrate that enstatite and water are miscible in all proportions if the temperature exceeds the melting point of MgSiO 3 . Furthermore, we performed smoothed particle hydrodynamics simulations to demonstrate that the conditions necessary for rock-water miscibility are reached during giant impacts between water-rich bodies of 0.7–4.7 Earth masses. Our simulations lead to water worlds that include a mixed layer of rock and water.

79 ASTRONOMY AND ASTROPHYSICS↗
NASA NTRS2002

Morphological Evolution and Weak Interface Development within CVD-Zirconia Coating Deposited on Hi-Nicalon Fiber

The phase contents and morphology of a ZrO2 fiber coating deposited at 1050 C on Hi-Nicalon(Tm) by chemical vapor deposition were examined as a function of deposition time from 5 to 120 min. The morphological evolution in the ZrO2 coating was correlated to the development of delamination within the ZrO2 coating. The delamination appears to occur as a result of: (1) continuous formation of tetragonal ZrO2 nuclei on the deposition surface; (2) martensitic transformation of the tetragonal phase to a monoclinic phase upon reaching a critical grain size; and (3) development of significant compressive hoop stresses due to the volume dilation associated with the transformation. Our observations suggest that it will be of critical importance to further understand and eventually control the nucleation and grain growth behavior of CVD ZrO2 and its phase transformation behavior for its potential applications for composites.

Li, Hao↗
NASA NTRS2006

Fundamental Properties of O-Type Stars

We present a comprehensive analysis of high-resolution, far-ultraviolet HST STIS, FUSE, and optical spectra of 18 O stars in the Small Magellanic Cloud. Our analysis is based on the OSTAR2002 grid of NLTE metal-line-blanketed model atmospheres calculated with our code TLUSTY. We systematically explore and present the sensitivity of various UV and optical lines to different stellar parameters. We have obtained consistent fits of the UV and the optical spectrum to derive the effective temperature, surface gravity, surface composition, and microturbulent velocity of each star. Stellar radii, masses, and luminosities follow directly. For stars of the same spectral subtype, we find a general good agreement between effective temperature determinations obtained with TLUSTY, CMFGEN, and FASTWIND models, which are all lower than the standard T(sub eff) calibration of O stars. We propose a new calibration between the spectral type and effective temperature based on our results from UV metal lines, as well as optical hydrogen and helium lines. The lower effective temperatures translate into ionizing luminosities that are smaller by a factor of 3 compared to luminosities inferred from previous standard calibrations. The chemical composition analysis reveals that the surface of about 80% of the program stars is moderately to strongly enriched in nitrogen, while showing the original helium, carbon, and oxygen abundances. Our results support the new stellar evolution models that predict that the surface of fast rotating stars becomes nitrogen-rich during the main-sequence phase because of rotationally induced mixing. Enrichment factors are, however, larger than predicted by stellar evolution models. Most stars exhibit the "mass discrepancy" problem, which we interpret as a result of fast rotation that lowers the measured effective gravity. Nitrogen enrichment and low spectroscopic masses are therefore two manifestations of fast rotation. Our study thus emphasizes the importance of rotation in our understanding of the properties of massive stars and provides a framework for investigating populations of low-metallicity massive stars at low and high redshifts.

Heap, Sara R.↗
NASA NTRS2022

Ultraviolet Spectropolarimetry Conservative and Nonconservative Mass Transfer in OB Interacting Binaries

The current consensus is that at least half of the OB stars are formed in binary or multiple star systems. The evolution of OB stars is greatly influenced by whether the stars begin as close binaries, and the evolution of the binary systems depend on whether the mass transfer is conservative or nonconservative. FUV/NUV spectropolarimetry is poised to answer the latter question. This paper discusses how the Polstar spectropolarimetry mission can characterize the degree of nonconservative mass transfer that occurs at various stages of binary evolution, from the initial mass reversal to the late Algol phase, and quantify its amount. The proposed instrument combines spectroscopic and polarimetric capabilities, where the spectroscopy can resolve Doppler shifts in UV resonance lines with 10 km/s precision, and polarimetry can resolve linear polarization with 10 −3 precision or better. The spectroscopy will identify absorption by mass streams and other plasmas seen in projection against the stellar disk as a function of orbital phase, as well as scattering from extended splash structures, including jets. The polarimetry tracks the light coming from material not seen against the stellar disk, allowing the geometry of the scattering to be tracked, resolving ambiguities left by the spectroscopy and light-curve information. For example, nonconservative mass streams ejected in the polar direction will produce polarization of the opposite sign from conservative transfer accreting in the orbital plane. Time domain coverage over a range of phases of the binary orbit are well supported by the Polstar observing strategy. Special attention will be given to the epochs of enhanced systemic mass loss that have been identified from IUE observations (pre-mass reversal and tangential gas stream impact). We show how the history of systemic mass and angular momentum loss/gain episodes can be inferred via ensemble evolution through the r–q diagram. Combining the above elements will significantly improve our understanding of the mass transfer process and the amount of mass that can escape from the system, an important channel for changing the final mass and ultimate supernova of a large number of massive stars found in binaries at close enough separation to undergo interaction.

Geraldine J. Peters↗
NASA NTRS1993

Discovery of Orbital Decay in SMC X-1

We report on the results of three observations of the binary X-ray pulsar SMC X-1 with the Ginga satellite. Timing analyses of the 0.71 s X-ray pulsations yield Doppler delay curves which, in turn, enable the most accurate determination of the SMC X-1 orbital parameters available to date. Epochs of phase zero for the 3.9 day orbit were determined for 1987 May, 1988 August, and 1989 August with accuracies of 13, 0.6, and 3 s, respectively. These epochs are combined with two previous determinations of the orbital epoch to yield the rate of change in the orbital period dot-P(orb)/P(orb) = ( 3.36 +/- 0.02) x 10(exp -6) yr(exp -1). An interpretation of the orbital decay is made in the context of tidal evolution, with consideration of the influence of the increasing moment of inertia of the companion star due to its nuclear evolution. We find that, while the orbital decay is probably driven by tidal interactions, the asynchronism between the orbit and the rotation of the companion star is most likely maintained by the evolutionary expansion of the companion star (Sk 160) rather than via the Darwin instability. In this case Sk 160 is likely to be in the hydrogen shell burning phase of its evolution. Finally, a discussion is presented of the relation among the time scales for stellar evolution (less than 10(exp 7) yr), orbital decay (3 x 10(exp 5) yr), and neutron-star spin-up in the SMC X-1 system (2000 yr). In particular, we present the result of a self-consistent calculation for the histories of the spin of the neutron star and the mass transfer in this system. A plausible case can be made for the spin-up time scale being directly related to the lifetime of the luminous X-ray phase which will end in a common-envelope phase within a time of less than approx. 10(exp 4) yr.

Levine, A.↗
NASA NTRS1992

Modeling of coalescence, agglomeration, and phase segregation in microgravity processing of bimetallic composite materials

The overall objective of this research is to develop models to predict drop-size-distribution evolutions due to droplet collisions and coalescence during processing within the miscibility gap of bimetallic liquid-phase-miscibility-gap materials. The individual and collective action of gravitational and nongravitational mechanisms on the relative motion and coalescence of drops are considered.

Davis, Robert H.↗
NASA NTRS1999

A View of the Lunar Interior Through Lunar Laser Range Analysis

Laser ranges between observatories on the Earth and retroreflectors on the Moon started in 1969 and continue to the present. Recent range accuracies are 2 cm while earliest ranges are an C, order of magnitude less certain. Four retroreflectors are ranged: three located at the Apollo 11, 14, and 15 sites and one on the Lunakhod 2 rover. Accurate analysis of the range data determines a number of lunar science parameters. The lunar interior variables include a fluid core parameter. The Lunar Laser Ranging effort is reviewed elsewhere. Many parameters are detected through their influence on rotation. Also detected are solid-body tides and accurate selenocentric reflector locations. Determined through the rotation are moment-of-inertia differences, gravitational harmonics, potential Love number, and dissipation effects due to tides and molten core. The rotation of the Moon is not at its minimum energy state; some recently active process has caused free librations. The moment differences contributed to the recent improvement of the Moon's moment of inertia from the Lunar Prospector gravity field. The Love numbers provide bulk elastic properties. Future possibilities for measurement include oblateness of the core-mantle boundary and core moment. A study of dissipation signatures in the rotation determines tidal Q vs. frequency and concludes that the Moon has a molten core. At 1 month the tidal Q is 37 and at 1 yr it is 60. The core radius is < or = 352 km for Fe and < or = 374 km for the Fe-FeS eutectic. The core detection exceeds 3x its uncertainty. The spin of the core is not aligned with the spin of the mantle and torque arises from the velocity difference at the boundary. Yoder's turbulent boundary layer theory is used to compute the radii. The present heat generation from tides and core interaction is minor compared to radiogenic heating. The heating for ancient times is more interesting. Peale and Cassen investigated lunar tidal heating while the lunar orbit expanded due to tides on Earth. Their calculations predate the measurement of Q and should be multiplied by 3.45 to match the lunar-laser-determined Love number and monthly Q. Tidal-heating computations depend on how fast the lunar orbit evolved and whether the tidal dissipation is localized. Neither is known, but plausible assumptions lead to early central region temperature increases of several hundred degrees. Most of the energy is deposited early in the Moon's history. The turbulent boundary layer theory allows a prediction of energy dissipated at the core-mantle boundary during orbit evolution. Under the assumption that the properties of the early core are the same as at present, the energy dissipated by core-mantle interaction is about the same as for tidal dissipation, but it is deposited in a smaller volume. This source of energy is capable of promoting convection in an early fluid core and driving a dynamo. This is a transient phase with a duration depending on the rate of orbit evolution. Plausible assumptions lead to a duration of a few hundred million years. Thus, the remnant magnetization of many lunar rocks is compatible with a brief global magnetic field powered by dynamical energy dissipation. Analysis of the lunar laser ranges is providing information on lunar geophysics. Future data will improve accuracies of present solution parameters, and several more interior effects should be detectable.

Williams, J. G.↗
DOE OSTI2026

Phase Transitions of Eutectic High Entropy Alloy AlCoCrFeNi 2.1 Under Shock Compression

High entropy alloys (HEAs) are a new class of metals that exhibit unique mechanical performance. Among HEAs, additively manufactured eutectic high entropy alloys (AM EHEAs) have recently emerged as candidate materials for use in extreme conditions due to their simultaneous high strength and ductility. However, the deformation and structural evolution of AM EHEAs under conditions of high pressure have not been well characterized, limiting their use in extreme applications. Dynamic compression experiments and molecular dynamics simulations are presented to study the structural evolution of AM EHEA AlCoCrFeNi 2.1 when compressed to pressures up to 400 GPa. In situ X-ray diffraction measurements capture the appearance of face-centered cubic and body-centered cubic phases at different pressure conditions, with pure- and mixed-phase regions. Furthermore, understanding the phase stability and structural evolution of the AM EHEA offers new insights to guide the development of high-performance complex materials for extreme conditions.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Influence of the Molecular Structure on the Electrocatalytic Hydrogenation of Carbonyl Groups and H 2 Evolution on Pd

We investigated the electrocatalytic hydrogenation (ECH) of model aldehydes and ketones over carbon supported Pd in aqueous phase. We propose reaction mechanisms based on kinetic measurements and on spectroscopic and electrochemical characterization of the working catalyst. The reaction rates of ECH and of the H 2 evolution reaction (HER) vary with the applied electric potential following trends that strongly depend on the organic substrate. The intrinsic rates of hydrogenation and H 2 evolution are influenced, in opposing ways, by the sorption of the reacting organic substrate. Strong interactions, i.e., higher standard free energies of adsorption of the organic compound, induce high hydrogenation rates but decrease the overall currents. The fast hydrogenation kinetics produces a hydrogen-depleted environment that kinetically hinders the HER and the bulk phase transition of Pd to a H-rich bulk Pd hydride, which is triggered by the applied potential in the absence of reacting organic compounds. As consequence of strong organic-metal interactions, hydrogenation dominates at low overpotential. However, the coverages of organic substrates on the metal surface decrease and the rates of H 2 evolution surpass those of hydrogenation with increasingly negative electric potential. We determined the range of electric potential favoring hydrogenation on Pd and quantitatively deconvoluted the effects of the sorption of the organic compound, and of the rates of proton coupled electron transfers, on the kinetics of both ECH and HER. The results indicate that electrocatalysis offers hydrogenation pathways for polar molecules that are different and, in some cases, faster than those dominating in the absence of an external electric potential.

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

Small-scale mechanical testing and characterization of fuel cladding chemical interaction between HT9 cladding and advanced U-based metallic fuel alloy

Fuel cladding chemical interactions (FCCI) occurred on the interface between the nuclear metal fuel and cladding is the primary cause of cladding wastage, weakening cladding mechanical integrity, and placing fuel and cladding at risk. Although the microstructural and phase information of FCCI has been fairly understood, mechanical properties remain less studied due to limited reaction volume. Here, through a combining of advanced electron microscopy characterizations and small-scale mechanical testing techniques, including indentation and micro-tensile testing, this study investigated the microscale mechanical properties of FCCI between the ferritic/martensitic (F/M) HT9 cladding and an advanced Uranium (U)-based metallic fuel irradiated at the Advanced Test Reactor to 2.2% FIMA with peak inner cladding temperature reached to 650 °C. Mechanical testing results show significant hardening and embrittlement in the FCCI region. The brittle fracture of FCCI specimen is mainly attributed to the formation of nano-crystallized intermetallic σ-FeCr phase. Whereas mechanical softening was revealed in the unreacted HT9 matrix due to irradiation-induced microstructural and microchemical evolution, specifically, the disappearance of martensitic lath structure and the formation of Fe 2 Mo Laves phase precipitation which consumed the solid solution strengthening Mo from the F/M HT9 matrix. Due to the achieved high cladding temperature, this fuel pin is of particular significance for revealing the high-temperature irradiation effect on the mechanical properties of HT9 cladding. Therefore, the outcomes of this study are expected to contribute to the development of multi-scale mechanical behavior modeling of HT9 cladding for Generation IV reactors which requires cladding to run at higher temperature (above 600 ?).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Compositional heterogeneity in Cs y FA 1- y Pb(Br x I 1- x ) 3 perovskite films and its impact on phase behavior

Hybrid organic inorganic lead halide perovskite semiconductors of the form Cs y FA 1-y Pb(Br x I 1-x ) 3 are promising candidate materials for high-efficiency photovoltaics. Notably, cation and anion substitution can be used to tune the band gaps to optimize performance and improve stability. However, multi-component materials can be prone to compositional and structural inhomogeneity and the extent, length scale and impact of this heterogeneity on lead halide perovskite properties are not well understood. Here we use synchrotron X-ray diffraction to probe the evolution of crystal structure across the tetragonal-to-cubic phase transition for a series of Cs y FA 1-y Pb(Br x I 1-x ) 3 thin films with x = 0.05 to 0.3 and y = 0.17 to 0.40. We find that the transition occurs across a broad temperature range of approximately 40 °C, much larger than for pure compounds such as MAPbI 3 and MAPbBr 3 . Finally, we hypothesize that this smearing of the phase transition is due to compositional inhomogeneities that give rise to a distribution of local transition temperatures and we estimate the composition varies by about 10% to 15% with likely greater heterogeneity for the halide anion than the cation. This approach of mapping the transition is a simple and effective method of assessing heterogeneity, enabling evaluation of its impact.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Evolution of silicate coordination in architected amorphous and crystalline magnesium silicates during carbon mineralization

Advancing durable solutions for carbon storage and removal at the gigaton scale to produce solid carbonates via carbon mineralization requires harnessing earth abundant magnesium silicate resources. Calibrated insights linking the structural and morphological features of earth abundant amorphous and crystalline magnesium silicate phases to their reactivity are essential for scalable deployment but remain underdeveloped. To resolve the influence of silica coordination and mass transfer on carbon mineralization behavior, magnesium silicates bearing amorphous and crystalline phases (AC Mg-silicate) are synthesized. The structural and morphological transitions starting from colloidal precursors to their final synthesized form on heating are delineated using operando ultra small/small/wide angle X-ray scattering (USAXS/SAXS/WAXS) measurements. The evolution of the silicate phases on carbon mineralization of AC Mg-silicate is contrasted with that of highly crystalline Mg-silicate (HC Mg-silicate) when reacted at 200 °C and a CO 2 partial pressure of 20 atm in water and 1 M NaHCO 3 solution in stirred and unstirred environments. These experimental conditions are analogous to those of the water–gas-shift reaction for sustainable recovery of H 2 with inherent carbon mineralization. Enhancement in the extent of carbon mineralization by 13.3–19.5% noted in the presence of NaHCO 3 compared to water in AC and HC Mg-silicate with and without stirring, is attributed to the buffering effect which aids simultaneous silicate dissolution and carbon mineralization. Enhanced extents of carbon mineralization in the presence of NaHCO 3 correspond to the formation of MgSiO 3 and SiO 2 phases from the starting Mg 2 SiO 4 precursors in AC and HC Mg-silicate. Unlocking these silicate transformations during carbon mineralization by harnessing architected Mg-silicate precursors reveals the feasibility of integrating these chemical pathways with sustainable H 2 conversion pathways with inherent carbon mineralization.

Gao, Xun [Cornell Univ., Ithaca, NY (United States↗
DOE OSTI2024

Finite-Time Teleportation Phase Transition in Random Quantum Circuits

How long does it take to entangle two distant qubits in a quantum circuit evolved by generic unitary dynamics? Here, we show that if the time evolution is followed by measurements of all but two infinitely separated test qubits, then the entanglement between them can undergo a phase transition and become nonzero at a finite critical time t c . The fidelity of teleporting a quantum state from an input qubit to an infinitely distant output qubit shows the same critical onset. Specifically, these finite-time transitions occur in short-range interacting two-dimensional random unitary circuits and in sufficiently long-range interacting one-dimensional circuits. The phase transition is understood by mapping the random continuous-time evolution to a finite-temperature thermal state of an effective spin Hamiltonian, where the inverse temperature equals the evolution time in the circuit. In this framework, the entanglement between two distant qubits at times t > t c corresponds to the emergence of long-range ferromagnetic spin correlations below the critical temperature. We verify these predictions using numerical simulation of Clifford circuits and propose potential realizations in existing platforms for quantum simulation.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Primordial black holes from bubble collisions during a first-order phase transition

We study the possibility of production of primordial black holes (PBHs) from bubble collisions during a first-order phase transition. While typical colliding bubbles are small and irrelevant for PBH production, we find that those that can produce PBHs must have a macroscopically thick fluid shell and have been born much before the typical nucleation time. Particularly large uncertainties arise from an exponential sensitivity of the nucleation rate on the required duration of bubble growth which depends on the details of the collisions and the evolution of the spacetime metric toward the end of the phase transition. We introduce a few parameters to be obtained from future numerical simulation to represent those unknowns, and estimate the PBH abundance in an Abelian Higgs benchmark model and show that it can be significant. We predict an approximately monochromatic PBH mass spectrum, and find regions in the parameter space where the PBHs can constitute entire dark matter or even overclose the Universe. Our result thus shows that models with a first-order phase transition can be constrained by overabundant PBHs or null results of other PBH searches. Published by the American Physical Society 2024

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Chemical and Structural Evolution of AgCu Catalysts in Electrochemical CO 2 Reduction

Silver–copper (AgCu) bimetallic catalysts hold great potential for electrochemical carbon dioxide reduction reaction (CO 2 RR), which is a promising way to realize the goal of carbon neutrality. Although a wide variety of AgCu catalysts have been developed so far, it is relatively less explored how these AgCu catalysts evolve during CO 2 RR. The absence of insights into their stability makes the dynamic catalytic sites elusive and hampers the design of AgCu catalysts in a rational manner. Here, in this study, we synthesized intermixed and phase-separated AgCu nanoparticles on carbon paper electrodes and investigated their evolution behavior in CO 2 RR. Our time-sequential electron microscopy and elemental mapping studies show that Cu possesses high mobility in AgCu under CO 2 RR conditions, which can leach out from the catalysts by migrating to the bimetallic catalyst surface, detaching from the catalysts, and agglomerating as new particles. Besides, Ag and Cu manifest a trend to phase-separate into Cu-rich and Ag-rich grains, regardless of the starting catalyst structure. The composition of the Cu-rich and Ag-rich grains diverges during the reaction and eventually approaches thermodynamic values, i.e., Ag 0.88 Cu 0.12 and Ag 0.05 Cu 0.95 . The separation between Ag and Cu has been observed in the bulk and on the surface of the catalysts, highlighting the importance of AgCu phase boundaries for CO 2 RR. In addition, an operando high-energy-resolution X-ray absorption spectroscopy study confirms the metallic state of Cu in AgCu as the catalytically active sites during CO 2 RR. Taken together, this work provides a comprehensive understanding of the chemical and structural evolution behavior of AgCu catalysts in CO 2 RR.

Chen, Peng-Cheng↗