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We study the influence of the liquid-vapor surface on the crystallizationkinetics of supercooled metal alloys. While a good glass former,$\rm{Cu}_{50}\rm{Zr}_{50}$, shows no evidence of surface enhancement ofcrystallization, $\rm{Ni}_{50}\rm{Al}_{50}$ exhibits an increased rate ofcrystallization due to heterogeneous nucleation at the free liquid surface. Thedifference in the compositional fluctuations at the interface is proposed asthe explanation of the distinction between the two alloys. Specifically, weobserve compositional ordering at the surface of $\rm{Ni}_{50}\rm{Al}_{50}$while the $\rm{Cu}_{50}\rm{Zr}_{50}$ alloy only exhibits a diffuse adsorptionof the Cu at the interface. We argue that the general difference in compositionsusceptibilities at planar surfaces represents an important factor inunderstanding the difference in the glass forming ability of the two alloys.

Chemical Ordering and Crystal Nucleation at the Liquid Surface: A Comparison of $\rm{Cu}_{50}\rm{Zr}_{50}$ and $\rm{Ni}_{50}\rm{Al}_{50}$ Alloys