Abstract

The surface of a glassy material exhibits enhanced mobility compared to the bulk counterpart, however the underlying mechanism for this remains elusive. Herein, we present studies of the dynamical properties of a prototypical glass-forming metallic liquid ${\mathrm{Zr}}_{50}{\mathrm{Cu}}_{50}$ as a function of the distance from both the free surface and pinned surface using molecular dynamics simulations. We found that the surface mobility increases gradually on approaching the free surface, with a concomitant increase of the non-Gaussianity. The phonon density of states at the free surface exhibits lower characteristic frequencies than in the bulk and pinned surface. These results suggest phonon softening caused by anisotropic fluctuations at free surfaces as an alternative physical mechanism leading to the enhanced dynamics at free glassy surfaces from the perspective of collective excitations.

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