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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 37 records · Page 2

Quantifying disorder one atom at a time using an interpretable graph neural network paradigm

Abstract Quantifying the level of atomic disorder within materials is critical to understanding how evolving local structural environments dictate performance and durability. Here, we leverage graph neural networks to define a physically interpretable metric for local disorder, called SODAS. This metric encodes the diversity of the local atomic configurations as a continuous spectrum between the solid and liquid phases, quantified against a distribution of thermal perturbations. We apply this methodology to four prototypical examples with varying levels of disorder: (1) grain boundaries, (2) solid-liquid interfaces, (3) polycrystalline microstructures, and (4) tensile failure/fracture. We also compare SODAS to several commonly used methods. Using elemental aluminum as a case study, we show how our paradigm can track the spatio-temporal evolution of interfaces, incorporating a mathematically defined description of the spatial boundary between order and disorder. We further show how to extract physics-preserved gradients from our continuous disorder fields, which may be used to understand and predict materials performance and failure. Overall, our framework provides a simple and generalizable pathway to quantify the relationship between complex local atomic structure and coarse-grained materials phenomena.

36 MATERIALS SCIENCE↗

High Entropy Alloys: Irradiation

High entropy alloys (HEAs) have been considered as structural materials for nuclear applications due to their promising mechanical properties and radiation resistance. For this purpose, irradiation-induced defect evolution and microstructure change have been characterized to evaluate the irradiation performance of different HEAs. This article reviews recent advances in understanding the irradiation response of HEAs, including the effect of disordered states on the defect energy landscape and defect evolution, irradiation-induced microstructure changes, void swelling, phase stability, mechanical properties under irradiation, as well as the He irradiation effects.

Zhao, Shijun↗

Understanding the local structure of disordered carbons from cellulose and lignin

An electron microscopy investigation was performed to understand the relationship between the microstructure and properties of carbonized cellulose and lignin (softwood kraft lignin) relative to the structure of the original biomass components. Structure details at micro- and molecular levels were investigated by scanning transmission electron microscopy. Atomic-resolution images revealed the presence of random disordered carbon in carbonized cellulose (C-CNC) and of large domains of well-ordered carbon with graphite sheet structure in carbonized lignin (C-Lignin). These structural differences explain why C-CNC exhibits higher surface area and porosity than C-Lignin. The presence of certain well-ordered carbon in carbonized lignin indicates some of the carbon in lignin are graphitized with heat treatment temperature up to 950 °C. This result is encouraging for future endeavors of attaining acceptable modulus of carbon fiber from lignin given suitable modifications to the chemistry and structure of lignin. The results of this research contribute to an improved understanding of the carbonization mechanism of the key cellulose and lignin components of biomass materials.

54 ENVIRONMENTAL SCIENCES↗

Unprecedented non-hysteretic superelasticity of [001]-oriented NiCoFeGa single crystals

Superelasticity associated with the martensitic transformation has found a broad range of engineering applications. However, the intrinsic hysteresis and temperature sensitivity of the first-order phase transformation significantly hinder the usage of smart metallic components in many critical areas. In this paper, we report a large superelasticity up to 15.2% strain in [001]-oriented NiCoFeGa single crystals, exhibiting non-hysteretic mechanical responses, a small temperature dependence and high-energy-storage capability and cyclic stability over a wide temperature and composition range. In situ synchrotron X-ray diffraction measurements show that the superelasticity is correlated with a stress-induced continuous variation of lattice parameter accompanied by structural fluctuation. Neutron diffraction and electron microscopy observations reveal an unprecedented microstructure consisting of atomic-level entanglement of ordered and disordered crystal structures, which can be manipulated to tune the superelasticity. The discovery of the large elasticity related to the entangled structure paves the way for exploiting elastic strain engineering and development of related functional materials. NiCoFeGa single crystals exhibit large non-hysteretic superelasticity over broad temperature and composition ranges. It is attributed to the continuous phase transition with applied stress, which is related to the fluctuation of entangled ordered and disordered crystal structures.

36 MATERIALS SCIENCE↗

Hybrid microstructure of smectite clay gels revealed using neutron and synchrotron X-ray scattering

Aqueous suspensions of swelling clays display a nematic sol-gel transition at very low solid concentrations. The underlying microstructure of the gel has remained a point of contention since the time of Irving Langmuir and has been a major obstacle to fully realizing the potential of clays for practical applications. Here, we comprehensively probe the microstructure of a smectite clay suspension using ultra-small angle neutron/X-ray scattering and find that the nematic gel is structurally ordered and contains entities that are at least an order of magnitude larger than the individual particles. Complementary cryo-electron microscopy shows the presence of domains having particle-particle ordering responsible for nematic texture and regions of particle-particle aggregation responsible for gel-like behavior. We find that the smectic clay gels have a hybrid microstructure with co-existing repulsive nematic domains and attractive disordered domains.

36 MATERIALS SCIENCE↗

Microstructural and rheological training and memory of nanocolloidal soft glasses under cyclic shear

An intrinsic feature of disordered and out-of-equilibrium materials, such as glasses, is the dependence of their properties on their history. An important example is rheological memory, in which disordered solids obtain properties based on their deformation history. Here, in this study, we employ x-ray photon correlation spectroscopy with in situ rheometry to characterize memory formation in a nanocolloidal soft glass due to cyclic shear. During a cycle, particles undergo irreversible displacements composed of a combination of shear-induced diffusion and heterogeneous, residual strain fields. At lower shear amplitudes, the displacements resemble a random walk in which the directions in each cycle are independent of those in preceding cycles, while at high amplitude, the irreversible displacements in consecutive cycles become correlated. The magnitudes of the displacements decrease with each cycle before reaching a steady state where the microstructure has been trained to achieve enhanced reversibility even at shear amplitudes well above yielding and despite the presence of thermal fluctuations. At amplitudes below and near yielding, these decreases are monotonic, while well above yielding, they are nonmonotonic, suggesting evidence of shear banding. Accompanying this microstructural training are corresponding decreases in the dissipation during each cycle and the magnitude of the residual stress toward steady-state values. Memory of the training is revealed by measurements in which the amplitude of the shear is changed after steady state is reached. The magnitude of the particle displacements, as well as the dissipation and the change in residual stress, vary nonmonotonically with the new shear amplitude, having minima near the training amplitude, thereby revealing correlated microscopic and macroscopic signatures of memory.

Chen, Yihao [Johns Hopkins Univ., Baltimore, MD (U↗

Low-threshold supercontinuum generation in polycrystalline media

Until recently, the generation of super-octave continua in bulk materials at full repetition rates of femtosecond (fs) oscillators has been limited to a few special cases of Kerr lens mode-locked Ti:sapphire lasers. In 2019, we described a 3.4-octave fs source with 50 nJ pulse energy at the repetition rate of 78 MHz based on polycrystalline Cr:ZnS [Vasilyev et al. , Optica 6 , 126 ( 2019 ) OPTIC8 2334-2536 10.1364/OPTICA.6.000126 ]. Here we explain the mechanism of fs supercontinuum generation in transition-metal doped polycrystalline II-VI semiconductors at relatively low (nJ-level) pulse energy. We demonstrate that this new supercontinuum regime is enabled by a complex, yet well-reproducible, interplay between the effects arising from the third-order nonlinearity, the quadratic nonlinearities, and thermal optical effects in the medium. We also demonstrate the control of fs pulse propagation in disordered χ <#comment/> ( 2 ) media via the control of the material microstructure.

Vasilyev, Sergey (ORCID:0000000225203547)↗

High-temperature ordered intermetallic alloys II; Proceedings of the Second Symposium, Boston, MA, Dec. 2-4, 1986

The papers presented in this volume provide on overview of recent theoretical and experimental research in the field of high-temperature ordered intermetallic alloys. The papers are gouped under the following headings: ordering behavior and theory, microstructures, mechanical behavior, alloy design and microstructural control, and metallurgical properties. Specific topics discussed include antiphase domains, disordered films and the ductility of ordered alloys based on Ni3Al; kinetics and mechanics of formation of Al-Ni intermetallics; deformability improvements of L1(2)-type intermetallic compounds; B2 aluminides for high-temperature applications; and rapidly solidified binary TiAl alloys.

Stoloff, N. S.↗

Effects of rejuvenation modes on the microstructures and mechanical properties of metallic glasses

This study systematically investigates the effects of three rejuvenation modes, namely biaxial loading, thermal pressure loading, and cryogenic thermal cycling, on the microstructures and mechanical properties of Cu 64 Zr 36 metallic glasses (MGs) using molecular dynamics (MD) simulations. The simulation results demonstrate that biaxial tension application during loading results in a rejuvenated glassy state with high strength. Specifically, we find that the yield stress, Young's modulus, and shear modulus of the rejuvenated glass obtained by biaxial tensile loading decreased by 2.8%, 2.1%, and 2.7%, respectively, compared to an as-cast MG reference. We also find that MGs achieve the greatest degree of rejuvenation, at the expense of strength, with the use of thermal pressure loading. Interestingly, the application of cryogenic thermal cycling results in a rejuvenated state with a lower strength drop compared to thermal pressure loading. Furthermore, analysis of the potential energy and medium-range-order (MRO) size indicates that the microstructures of MGs achieves a high-energy ordered glass state after thermal pressure loading, but a high-energy disordered glass state after biaxial tensile loading and cryogenic thermal cycling. Furthermore, these findings provide meaningful insights into the effect of rejuvenation modes on the microstructures and mechanical properties of MGs, as well as useful guidelines for designing MGs with high strength and superior plasticity for prospective applications in industry.

36 MATERIALS SCIENCE↗

Coexistence of ordered and disordered vacancies in tungsten diboride with a broken hexagonal symmetry

As an important member of transition-metal borides, tungsten diboride (i.e., WB 2+𝑥 ) contains complex atomic vacancies with the originally assigned hexagonal symmetries, exhibiting many fascinating properties such as superconductivity and superior hardness. However, due to the difficulties in exploring atomic vacancies of transition-metal borides, the actual structure and composition of WB 2+𝑥 have been long-standing unsettled issues, which have impeded in-depth understanding of its structural stability and origins of such extraordinary properties. Here, we report a systematic investigation of the crystal structure of high-pressure synthesized WB 2+𝑥 samples by combination of state-of-the-art diffraction techniques and microstructural observations, leading to the discovery of an unusual coexistence of both the ordered and disordered atomic vacancies in WB 2+𝑥 with a broken hexagonal symmetry that can be well described by a dual-phase model involving hP12-W 0.70 ⁢B 1.73 and P1-W 0.75⁢ B 1.64 . Superposition of thin sample layers with disordered vacancies along the [001] or [110] direction is revealed to produce ordered vacancies, rationalizing the observed size-dependent symmetry breaking. In conclusion, these findings not only provide solid foundations for studying the phase stability and properties of this boride but also give powerful insights into how the intricate atomic vacancies can influence crystal structures of transition-metal borides.

high pressure↗

A molecular dynamics survey study of impact-induced amorphization in yttria nanoparticles

The impact of a single yttria (Y 2 O 3 ) nanoparticle onto a yttria substrate was studied as a function of particle velocity (300–1200 m/s) and diameter (5–12 nm) for three particle orientations and two substrate orientations using molecular dynamics simulations. Impacts resulted in minimal dislocation motion but extensive disordering of the crystal lattice without approaching the melting temperature. The resulting amorphous microstructure was both precisely coincident with plastic strain and retained until the end of the simulation, suggesting a deformation mechanism of amorphization-facilitated viscous flow. Further analysis revealed that the degree of amorphization depended primarily on the impact velocity and secondarily on the orientations of the particle and substrate, with significant second-order effects from variable interactions.

74 ATOMIC AND MOLECULAR PHYSICS↗

Visualizing Crystallization Dynamics and Transformation Pathways of Disordered Rocksalt Oxides During Thermally Activated Sol–Gel Synthesis

Sol–gel synthesis is a wet-chemical processing route for fabricating functional materials with control over composition and microstructure at relatively low temperatures compared to conventional solid-state synthesis. While sol–gel process initiates with intermixed molecular precursors, the early-stage nucleation pathways are insufficiently understood. Here, in this study, the chemical and structural transformation of ion disordered rocksalt (DRX) Li 1.2 Mn 0.4 Ti 0.4 O 2 (LMTO), a promising cathode material for lithium batteries, is studied by multiscale characterizations. In situ heating transmission electron microscopy (TEM) using a liquid cell visualizes and identifies crystallization pathways at the nanoscale. While some regions follow a classical multi-step transition through thermodynamically stable intermediates, others exhibit a kinetic shortcut via a localized amorphous matrix to directly form the DRX structure. Macroscale Fourier transform infrared spectroscopy corroborates the findings and reveals that transition metal ions are more strongly incorporated into the acetate-coordinated network than lithium. Although in situ heating TEM captures diverse local transformation pathways, in situ synchrotron X-ray diffraction indicates that the macroscopic transformation proceeds predominantly through spinel LMTO and lithium titanates toward DRX-LMTO. The findings uncover the spatiotemporal chemical and structural transformations in sol–gel derived DRX-LMTO materials, and call for fine-tuning of such sol–gel chemistries to manipulate the crystallization pathways and achieve target material homogeneity more efficiently.

cathode material↗

A method for mapping submicron-scale crystallographic order/disorder applied to human tooth enamel

Tooth enamel, the outermost layer of human teeth, is a complex, hierarchically structured biocomposite. The details of this structure are important in multiple human health contexts, from understanding the progression of dental caries (tooth decay) to understanding the process of amelogenesis and related developmental defects. Enamel is composed primarily of long, nanoscale crystallites of hydroxyapatite that are bundled by the thousands to form micron-scale rods. Studies with transmission electron microscopy show the relationships between small groups of crystallites and X-ray diffraction characterize averages over many rods, but the direct measurement of variations in local crystallographic structure across and between enamel rods has been missing. Here, we describe a synchrotron X-ray-based experimental approach and a novel analysis method developed to address this gap in knowledge. A ~500-nm-wide beam of monochromatic X-rays in conjunction with a sample section only 1 μm in thickness enables 2D diffraction patterns to be collected from small well-separated volumes within the enamel microstructure but still probes enough crystallites (~300 per pattern) to extract population-level statistics on crystallographic features like lattice parameter, crystallite size, and orientation distributions. Furthermore, the development of a quantitative metric to characterize relative order and disorder based on the azimuthal autocorrelation of diffracted intensity enables these crystallographic measurements to be correlated with their location within the enamel microstructure (e.g., between rod and interrod regions). These methods represent a step forward in the characterization of human enamel and will elucidate the variation of the crystallographic structure across and between enamel rods for the first time.

crystallographic order/disorder↗

High temperature transition aluminas in gamma-Al2O3: Review

High temperature treated transition aluminas display adsorptive and catalytic properties that are in many ways comparable to those of their low temperature counterpart gamma-Al2O3. While being important industrial catalysts as well as catalytic supports, their very basic crystallographic and structural characteristics remain poorly understood and thus actively studied. In this review, we critically examine the crystallography and structural complexity of these materials. Specifically, we address the crystallography of delta- and theta-Al2O3 polymorphs and show how structural intergrowth and disorder are accommodated in these phases. The structural complexity at the scale of overall microstructure is also examined, and the challenges and recent progress in quantification of the structure at ensemble level are discussed. Most pertinently to catalysis, we review the surfaces properties of high temperature treated Al2O3 and discuss the implications for understanding attributes relevant to heterogeneous catalysis.

Kovarik, Libor↗

Quantification of High-Temperature Transition Al2O3 and Their Phase Transformations

High temperature exposure of ?-Al2O3 can lead to a series of polymorphic transformations, including the formation of ?-Al2O3 and ?-Al2O3. Quantification of the microstructure in the ?/?-Al2O3 formation range represents a formidable challenge as both phases accommodate a high degree of structural disorder. In this work, we explore the use of XRD recursive stacking formalism for quantification of high temperature transition aluminas. We formulate the recursive stacking methodology for modelling of disorder in ?-Al2O3 and twinning in ?-Al2O3 and show that explicitly accounting for the disorder is necessary to reliably model the XRD patterns of high temperature transition alumina. In the second part, we use the recursive stacking approach to study phase transformation during high temperature (1050 ºC) treatment. We show that the two different intergrowth modes of ?-Al2O3 have different transformation characteristics, and that a significant portion of ?-Al2O3 is stabilized with ?-Al2O3 even after prolonged high-temperature exposures. In discussions, we outline the limitation of the current XRD approach and discuss a possible multimodal XRD and NMR approach which can improve analysis of complex transition aluminas. This work was performed in the Wiley Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by DOEs Office of Biological and Environmental Research and located at PNNL. The work was supported by the U.S. Department of Energy (DOE), Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences.

Kovarik, Libor↗

Predicting and Controlling Corrosion (Abbreviated Final Report)

Corrosion accumulates significant replacement costs in the transportation, utility, manufacturing, and infrastructure sectors. It also underpins several of LLNL’s core missions in stockpile stewardship, defense, and energy security. Whereas most corrosion and aging models are empirically parameterized to describe well-defined conditions late in the reaction, the factors that determine the early stages of corrosion—during which mitigation could be most impactful— are poorly understood. This project addressed the critical need for new approaches to predict the kinetics of corrosion initiation based on firm physical and chemical understanding. The activities encompassed degradation of relevant metals in both hydrogen-rich and environmental corrosion scenarios. The team integrated state-of-the-art multiscale simulation, in situ characterization, and data science within three technical thrusts: hydriding of Ti alloys; aqueous corrosion of Al and Ni-Cr alloys; and degradation of additively manufactured 316L stainless steel. In each case, novel capabilities were developed to identify and track the impacts of key atomistic, compositional, and microstructural features on the metal systems. For hydriding, protocols were developed to tightly integrate multiscale models, advanced multimodal characterization, and machine learning to determine how hydrogen interacts with native passivating surface oxides and nucleates new undesired phases, shedding new light on the critical role of grain boundaries, interfaces, and atomically disordered regions. For aqueous corrosion, the project demonstrated methods to predict dissolution rates of metal surfaces in corrosive solutions, to measure and understand microstructural and grain orientation effects on corrosion susceptibility, and to investigate competing growth and dissolution kinetics of surface oxides. For additively manufactured metals, analysis using state-of-the-art microscopy techniques revealed the role of specific heterogeneities invoked during laser processing, including cellular structure, dislocations, and precipitates, on corrosion susceptibility. In addition to new capabilities and understanding, the project provided an avenue for workforce development, as well as key partnerships with stakeholders in corrosion science.

08 HYDROGEN↗

High entropy alloys with hexagonal close-packed structure derived from thin film combinatorial approach

A thin film combinatorial synthesis approach was utilized to develop a compositional and structural library for the OsRuWCo alloy system. The survey of this alloy space produced 24 unique compositions and their corresponding crystal structures, which represent a phase map where amorphous and single-phase hexagonal close-packed alloys were identified. Based on the identification of a promising candidate film region, a new high entropy alloy based on OsRuWCo, but with non-equiatomic composition, was synthesized in bulk form. The alloy exhibited a single-phase hexagonal close-packed structure in the as-cast state. Three derivatives from this system were also developed by considering the heat of mixing, atomic size, and binary solubility. These new alloys are based on OsRuWCoIr and OsRuWCoFe, both of which exhibit single-phase hexagonal close-packed as-cast structures, as determined by X-ray diffraction and electron microscopy. Additionally, this large compositional space was utilized to evaluate conventional parameters that describe high entropy alloys (ΔS mix , ΔH mix , Ω, δ, and VEC), and these were found to elucidate the criteria for solid solution formation in this system. Additionally, trends illustrating the evolution from amorphous to crystalline phases are demonstrated and discussed. It is concluded that in this particular case, the dominant factors promoting crystallinity are thermodynamic or electronic, rather than geometric.

36 MATERIALS SCIENCE↗