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When a liquid is cooled well below its melting temperature at a rate that exceeds the critical cooling rate Rc, the crystalline state is bypassed and a metastable, amorphous glassy state forms instead. Rc (or the corresponding critical casting thickness dc) characterizes the glass-forming ability (GFA) of each material. While silica is an excellent glass-former with small Rc < 10-2 K/s, pure metals and most alloys are typically poor glass-formers with large Rc > 1010 K/s. Only in the past thirty years have bulk metallic glasses (BMGs) been identified with Rc approaching that for silica. Recent simulations have shown that simple, hard-sphere models are able to identify the atomic size ratio and number fraction regime where BMGs exist with critical cooling rates more than 13 orders of magnitude smaller than those for pure metals. However, there are a number of other features of interatomic potentials beyond hard-core interactions. How do these other features affect the glass-forming ability of BMGs? In this manuscript, we perform molecular dynamics simulations to determine how variations in the softness and non-additivity of the repulsive core and form of the interatomic pair potential at intermediate distances affect the GFA of binary alloys. These variations in the interatomic pair potential allow us to introduce geometric frustration and change the crystal phases that compete with glass formation. We also investigate the effect of tuning the strength of the many-body interactions from zero to the full embedded atom model on the GFA for pure metals. We then employ the full embedded atom model for binary BMGs and show that hard-core interactions play the dominant role in setting the GFA of alloys, while other features of the interatomic potential only change the GFA by one to two orders of magnitude. Despite their perturbative effect, understanding the detailed form of the intermetallic potential is important for designing BMGs with cm or greater casting thickness. [ABSTRACT FROM AUTHOR]

The likelihood that an undercooled liquid vitrifies or crystallizes depends on the cooling rate R. The critical cooling rate Rc, below which the liquid crystallizes upon cooling, characterizes the glass-forming ability (GFA) of the system. While pure metals are typically poor glass formers with Rc > 1012 K/s, specific multi-component alloys can form bulk metallic glasses (BMGs) even at cooling rates below R ~ 1 K/s. Conventional wisdom asserts that metal alloys with three or more components are better glass formers (with smaller Rc) than binary alloys. However, there is currently no theoretical framework that provides quantitative predictions for Rc for multi-component alloys. In this manuscript, we perform simulations of ternary hard-sphere systems, which have been shown to be accurate models for the glass-forming ability of BMGs, to understand the roles of geometric frustration and demixing in determining Rc. Specifically, we compress ternary hard sphere mixtures into jammed packings and measure the critical compression rate, below which the system crystallizes, as a function of the diameter ratios sB/sA and sC/sA and number fractions xA, xB, and xC. We find two distinct regimes for the GFA in parameter space for ternary hard spheres. When the diameter ratios are close to 1, such that the largest (A) and smallest (C) species are well-mixed, the GFA of ternary systems is no better than that of the optimal binary glass former. However, when sC/sA ≲ 0.8 is below the demixing threshold for binary systems, adding a third component B with sC < sB < sA increases the GFA of the system by preventing demixing of A and C. Analysis of the available data from experimental studies indicates that most ternary BMGs are below the binary demixing threshold with sC/sA < 0.8. [ABSTRACT FROM AUTHOR]

Bulk metallic glasses (BMGs) are amorphous alloys with desirable mechanical properties and processing capabilities. To date, the design of new BMGs has largely employed empirical rules and trial-and-error experimental approaches. Ab initio computational methods are currently prohibitively slow to be practically used in searching the vast space of possible atomic combinations for bulk glass formers. Here, we perform molecular dynamics simulations of a coarse-grained, anisotropic potential, which mimics interatomic covalent bonding, to measure the critical cooling rates for metal-metalloid alloys as a function of the atomic size ratio σS/σL and number fraction xS of the metalloid species. We show that the regime in the space of σS/σL and xS where well-mixed, optimal glass formers occur for patchy and LJ particle mixtures, coincides with that for experimentally observed metal-metalloid glass formers. Thus, our simple computational model provides the capability to perform combinatorial searches to identify novel glass-forming alloys. [ABSTRACT FROM AUTHOR]