Atomic-level structure and structure–property relationship in metallic glasses

Bulk metallic glass (BMG) formers are multicomponent alloys that vitrify with remarkable ease during solidification. Technological interest in these materials has been generated by their unique properties, which often surpass those of conventional structural materials. The metastable nature of BMGs, however, has imposed a barrier to broad commercial adoption, particularly where the processing requirements of these alloys conflict with conventional metal processing methods. Research on the crystallization of BMG formers has uncovered novel thermoplastic forming (TPF)-based processing opportunities. Unique among metal processing methods, TPF utilizes the dramatic softening exhibited by a BMG as it approaches its glass-transition temperature and decouples the rapid cooling required to form a glass from the forming step. This article reviews crystallization processes in BMG former and summarizes and compares TPF-based processing methods. Finally, an assessment of scientific and technological advancements required for broader commercial utilization of BMGs will be made.

Processing of Bulk Metallic Glass

Geochimica et Cosmochimica Acta

Amorphous solids, or glasses, are distinguished from crystalline solids by their lack of long-range structural order. At the level of two-body structural correlations, glassformers show no qualitative change upon vitrifying from a supercooled liquid. Nonetheless the dynamical properties of a glass are so much slower that it appears to take on the properties of a solid. While many theories of the glass transition focus on dynamical quantities, a solid's resistance to flow is often viewed as a consequence of its structure. Here we address the viewpoint that this remains the case for a glass. Recent developments using higher-order measures show a clear emergence of structure upon dynamical arrest in a variety of glass formers and offer the tantalising hope of a structural mechanism for arrest. However a rigorous fundamental identification of such a causal link between structure and arrest remains elusive. We undertake a critical survey of this work in experiments, computer simulation and theory and discuss what might strengthen the link between structure and dynamical arrest. We move on to highlight the relationship between crystallisation and glass-forming ability made possible by this deeper understanding of the structure of the liquid state, and emphasize the potential to design materials with optimal glassforming and crystallisation ability, for applications such as phase-change memory. We then consider aspects of the phenomenology of glassy systems where structural measures have yet to make a large impact, such as polyamorphism (the existence of multiple liquid states), aging (the time-evolution of non-equilibrium materials below their glass transition) and the response of glassy materials to external fields such as shear.

The role of local structure in dynamical arrest

Aims. We studied the evolution of the abundance in interstellar dust species that originate in stellar sources and from condensation in molecular clouds in the local interstellar medium of the Milky Way. We determined from this the input of dust material to the Solar System. Methods. A one-zone chemical evolution model of the Milky Way for the elemental composition of the disk combined with an evolution model for its interstellar dust component similar to that of Dwek (1998) is developed. The dust model considers dust-mass return from AGB stars as calculated from synthetic AGB models combined with models for dust condensation in stellar outflows. Supernova dust formation is included in a simple parametrised form that is gauged by observed abundances of presolar dust grains with a supernova origin. For dust growth in the ISM, a simple method is developed for coupling this with disk and dust evolution models. Results. A chemical evolution model of the solar neighbourhood in the Milky Way is calculated, which forms the basis for calculating a model of the evolution of the interstellar dust population at the galactocentric radius of the Milky Way. The model successfully passes all standard tests for the reliability of such models. In particular the abundance evolution of the important dust-forming elements is compared with observational results for the metallicity-dependent evolution of the abundances for G-type stars from the solar neighbourhood. It is found that the new tables of Nomoto et al. (2006) for the heavy element production give much better results for the abundance evolution of these important elements than the widely used tables of Woosley & Weaver (1995). The time evolution for the abundance of the following dust species is followed in the model: silicate, carbon, silicon carbide, and iron dust from AGB stars and from supernovae, as well as silicate, carbon, and iron dust grown in molecular clouds. It is shown that the interstellar dust population is dominated by dust accreted in molecular clouds; stardust only forms a minor fraction. Most of the dust material entering the Solar System at its formation does not show isotopic abundance anomalies of the refractory elements, i.e., inconspicuous isotopic abundances do not point to a Solar System origin for dust grains. The observed abundance ratios of presolar dust grains formed in supernova ejecta and in AGB star outflows requires that, for the ejecta from supernovae, the fraction of refractory elements condensed into dust is 0.15 for carbon dust and is quite small (∼10 −4 ) for other dust species.

/pdf/evolution-of-interstellar-dust-and-stardust-in-the-solar-58xwc4sdba.pdf

Evolution of interstellar dust and stardust in the solar neighbourhood

The effect of phase separation on subsequent crystallization in Al88Gd6La2Ni4

Correlated transmission electron microscopy and secondary ion mass spectrometry with submicron spatial resolution (NanoSIMS) investigations of the same presolar graphites spherules from the Murchison meteorite were conducted, to link the isotopic anomalies with the mineralogy and chemical composition of the graphite and its internal grains. Refractory carbide grains (especially titanium carbide) are commonly found within the graphite spherules, and most have significant concentrations of Zr, Mo, and Ru in solid solution, elements primarily produced by s-process nucleosynthesis. The effect of chemical fractionation on the Mo/Ti ratio in these carbides is limited, and therefore from this ratio one can infer the degree of s-process enrichment in the gas from which the graphite condensed. The resulting s-process enrichments within carbides are large (~200 times solar on average), showing that most of the carbide-containing graphites formed in the mass outflows of asymptotic giant branch (AGB) stars. NanoSIMS measurements of these graphites also show isotopically light carbon (mostly in the 100 < 12C/13C < 400 range). The enrichment of these presolar graphites in both s-process elements and 12C considerably exceeds that astronomically observed around carbon stars. However, a natural correlation exists between 12C and s-process elements, as both form in the He intershell region of thermally pulsing AGB stars and are dredged up together to the surface. Their observation together suggests that these graphites may have formed in chemically and isotopically inhomogeneous regions around AGB stars, such as high-density knots or jets. As shown in the companion paper, a gas density exceeding that expected for smooth mass outflows is required for graphite of the observed size to condense at all in circumstellar environments, and the spatially inhomogeneous, high-density regions from which they condense may also be incompletely mixed with the surrounding gas. We have greatly expanded the available data set of presolar graphites (N = 847) and characterized them by their morphology (onion type and cauliflower type). This effort has also revealed two new, rare presolar phases (iron carbide and metallic osmium). Due to the peculiar gas composition needed to form these rare presolar grain types, the graphites containing them are more likely to originate in supernova outflows.

PRESOLAR GRAPHITE FROM AGB STARS: MICROSTRUCTURE AND s-PROCESS ENRICHMENT

http://presolar.wustl.edu/Laboratory_for_Space_Sciences/Publications_2005_files/Stadermann-GCA-05.pdf

Supernova graphite in the NanoSIMS: Carbon, oxygen and titanium isotopic compositions of a spherule and its TiC sub-components

Three taxa of theSolidago canadensis L. complex are recognized for the Great Plains region:S. canadensis L. var.scabra Torr. & Gray,S. canadensis L. var.gilvocanescens Rydb., andS. canadensis L. var.hargeri Fern. Confusion has resulted from the use of var.gilvocanescens for two different plants: a shortleaved prairie ecotype most closely related to var.scabra and a short-haired form ofS. canadensis var.hargeri. The name rightly belongs to the former.

Solidago Canadensis Complex of the Great plains

Transmission electron microscope (TEM) investigations have revealed Os, Ru, Mo-rich refractory metal nuggets within four different presolar graphites, from both the high-density (HD) Murchison (MUR) and low-density (LD) Orgueil (ORG) fractions. Microstructural and chemical data suggest that these are direct condensates from the gas, rather than forming later by exsolution. The presolar refractory metal nugget (pRMN) compositions are variable (e.g., from 8 < Os atom% < 77), but follow the same chemical fractionation trends as isolated refractory metal nuggets (mRMNs) previously found in meteorites (Berg et al. 2009). From these compositions one can infer a temperature of last equilibration with the gas of 1405-1810 K (e.g., Berg et al. (2009) at approximately 100 dyne cm 2 pressure), which implies that the host graphites form over roughly the same range (in agreement with predictions) and that the pRMNs are chemically isolated from the gas when captured by graphite. Further, the pRMN compositions give evidence that HD graphites form at a higher T than LD ones. Chemical and phase similarities with the isolated mRMNs suggest that the mRMNs also condense directly from a gas, although from the early solar nebula rather than a presolar environment. Although the pRMNs themselves are too small for detection of isotopic anomalies, NanoSIMS isotopic measurements of their host graphites confirm a presolar origin for the assemblages. The two pRMN-containing LD graphites show evidence of a supernova (SN) origin, whereas the stellar origins of the pRMNs in HD graphite are unclear, because only less-diagnostic 12 C enrichments are detectable (as is commonly true for HD graphites).

/pdf/refractory-metal-nuggets-within-presolar-graphite-first-3cix7w95lt.pdf

Refractory metal nuggets within presolar graphite: First condensates from a circumstellar environment

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