Spatially Heterogeneous Dynamics in a Metallic Glass Forming Liquid Imaged by Electron Correlation Microscopy

Abstract

Supercooled liquids exhibit spatial heterogeneity in the dynamics of their fluctuating atomic arrangements. The length and time scales of the heterogeneous dynamics are central to the glass transition and influence nucleation and growth of crystals from the liquid. We report direct experimental visualization of the spatially heterogeneous dynamics as a function of temperature in the supercooled liquid state of a Pt-based metallic glass, using electron correlation microscopy with sub-nanometer resolution. An experimental four point space-time intensity correlation function demonstrates a growing dynamic correlation length, $\xi$, upon cooling of the liquid toward the glass transition temperature. $\xi$ as a function of the relaxation time $\tau$ data are in the good agreement with the Adam-Gibbs, inhomogeneous mode coupling theory and random first order transition theory of the glass transition. The same experiments demonstrate the existence of a nanometer thickness near surface layer with order of magnitude shorter relaxation time than inside the bulk.

updated references updated method to extract correlation length from g4(Δr, Δt); conclusion favoring RFOT model is weakened, but other results are unchanged

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• Spatially Heterogeneous Dynamics in a Metallic Glass Forming Liquid Imaged by Electron Correlation Microscopy

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• Geometric indicators of local plasticity in glasses measured by scanning small-beam diffraction
• Compositional Trends in Surface Enhanced Diffusion in Lead Silicate Glasses
• Chain-length-dependent correlated molecular motion in polymers