Synthesis of single-component metallic glasses by thermal spray of nanodroplets on amorphous substrates

We show that single component metallic glasses can be synthesized by thermal spray coating of nanodroplets onto an amorphous substrate. We demonstrate this using molecular dynamics simulations of nanodroplets up to 30 nm that the spreading of the nanodroplets during impact on a substrate leads to sufficiently rapid cooling (10^(12)–10^(13) K/s) sustained by the large temperature gradients between the thinned nanodroplets and the bulk substrate. However, even under these conditions, in order to ensure that the glass transition outruns crystal nucleation, it is essential that the substrate be amorphous (eliminating sites for heterogeneous nucleation of crystallization)

Automated computation of materials properties

Materials informatics offers a promising pathway towards rational materials design, replacing the current trial-and-error approach and accelerating the development of new functional materials. Through the use of sophisticated data analysis techniques, underlying property trends can be identified, facilitating the formulation of new design rules. Such methods require large sets of consistently generated, programmatically accessible materials data. Computational materials design frameworks using standardized parameter sets are the ideal tools for producing such data. This work reviews the state-of-the-art in computational materials design, with a focus on these automated $\textit{ab-initio}$ frameworks. Features such as structural prototyping and automated error correction that enable rapid generation of large datasets are discussed, and the way in which integrated workflows can simplify the calculation of complex properties, such as thermal conductivity and mechanical stability, is demonstrated. The organization of large datasets composed of $\textit{ab-initio}$ calculations, and the tools that render them programmatically accessible for use in statistical learning applications, are also described. Finally, recent advances in leveraging existing data to predict novel functional materials, such as entropy stabilized ceramics, bulk metallic glasses, thermoelectrics, superalloys, and magnets, are surveyed.Comment: 25 pages, 7 figures, chapter in a boo

Rate dependent shear bands in a shear transformation zone model of amorphous solids

We use Shear Transformation Zone (STZ) theory to develop a deformation map for amorphous solids as a function of the imposed shear rate and initial material preparation. The STZ formulation incorporates recent simulation results [Haxton and Liu, PRL 99 195701 (2007)] showing that the steady state effective temperature is rate dependent. The resulting model predicts a wide range of deformation behavior as a function of the initial conditions, including homogeneous deformation, broad shear bands, extremely thin shear bands, and the onset of material failure. In particular, the STZ model predicts homogeneous deformation for shorter quench times and lower strain rates, and inhomogeneous deformation for longer quench times and higher strain rates. The location of the transition between homogeneous and inhomogeneous flow on the deformation map is determined in part by the steady state effective temperature, which is likely material dependent. This model also suggests that material failure occurs due to a runaway feedback between shear heating and the local disorder, and provides an explanation for the thickness of shear bands near the onset of material failure. We find that this model, which resolves dynamics within a sheared material interface, predicts that the stress weakens with strain much more rapidly than a similar model which uses a single state variable to specify internal dynamics on the interface.Comment: 10 pages, 13 figures, corrected typos, added section on rate strengthening vs. rate weakening material

Transforming mesoscale granular plasticity through particle shape

When an amorphous material is strained beyond the point of yielding it enters a state of continual reconfiguration via dissipative, avalanche-like slip events that relieve built-up local stress. However, how the statistics of such events depend on local interactions among the constituent units remains debated. To address this we perform experiments on granular material in which we use particle shape to vary the interactions systematically. Granular material, confined under constant pressure boundary conditions, is uniaxially compressed while stress is measured and internal rearrangements are imaged with x-rays. We introduce volatility, a quantity from economic theory, as a powerful new tool to quantify the magnitude of stress fluctuations, finding systematic, shape-dependent trends. For all 22 investigated shapes the magnitude $s$ of relaxation events is well-fit by a truncated power law distribution $P(s)\sim {s}^{-\tau} exp(-s/s^*)$, as has been proposed within the context of plasticity models. The power law exponent $\tau$ for all shapes tested clusters around $\tau=$ 1.5, within experimental uncertainty covering the range 1.3 - 1.7. The shape independence of $\tau$ and its compatibility with mean field models indicate that the granularity of the system, but not particle shape, modifies the stress redistribution after a slip event away from that of continuum elasticity. Meanwhile, the characteristic maximum event size $s^*$ changes by two orders of magnitude and tracks the shape dependence of volatility. Particle shape in granular materials is therefore a powerful new factor influencing the distance at which an amorphous system operates from scale-free criticality. These experimental results are not captured by current models and suggest a need to reexamine the mechanisms driving mesoscale plastic deformation in amorphous systems.Comment: 11 pages, 8 figures. v3 adds a new appendix and figure about event rates and changes several parts the tex

The role of local structure in dynamical arrest

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.Comment: 70 page