Tuning the glass-forming ability of metallic glasses through energetic frustration

The design of multi-functional BMGs is limited by the lack of a quantitative understanding of the variables that control the glass-forming ability (GFA) of alloys. Both geometric frustration (e.g. differences in atomic radii) and energetic frustration (e.g. differences in the cohesive energies of the atomic species) contribute to the GFA. We perform molecular dynamics simulations of binary Lennard-Jones mixtures with only energetic frustration. We show that there is little correlation between the heat of mixing and critical cooling rate $R_c$, below which the system crystallizes, except that $\Delta H_{\rm mix} < 0$. By removing the effects of geometric frustration, we show strong correlations between $R_c$ and the variables $\epsilon_- = (\epsilon_{BB}-\epsilon_{AA})/(\epsilon_{AA}+\epsilon_{BB})$ and ${\overline \epsilon}_{AB} = 2\epsilon_{AB}/(\epsilon_{AA}+\epsilon_{BB})$, where $\epsilon_{AA}$ and $\epsilon_{BB}$ are the cohesive energies of atoms $A$ and $B$ and $\epsilon_{AB}$ is the pair interaction between $A$ and $B$ atoms. We identify a particular $f_B$-dependent combination of $\epsilon_-$ and ${\overline \epsilon}_{AB}$ that collapses the data for $R_c$ over nearly $4$ orders of magnitude in cooling rate.