Local structure in deeply supercooled liquids exhibits growing lengthscales and dynamical correlations

James E. Hallett, Francesco Turci, C. Patrick Royall*

*Corresponding author for this work

Research output: Contribution to journalArticle (Academic Journal)peer-review

37 Citations (Scopus)
212 Downloads (Pure)

Abstract

Glasses are among the most widely used of everyday materials, yet the process by which a liquid’s viscosity increases by 14 decades to become a glass remains unclear, as often contradictory theories provide equally good descriptions of the available data. Knowledge of emergent lengthscales and higher-order structure could help resolve this, but this requires time-resolved measurements of dense particle coordinates—previously only obtained over a limited time interval. Here we present an experimental study of a model colloidal system over a dynamic window significantly larger than previous measurements, revealing structural ordering more strongly linked to dynamics than previously found. Furthermore we find that immobile regions and domains of local structure grow concurrently with density, and that these regions have low configurational entropy. We thus show that local structure plays an important role at deep supercooling, consistent with a thermodynamic interpretation of the glass transition rather than a principally dynamic description.

Original languageEnglish
Article number3272
Number of pages10
JournalNature Communications
Volume9
DOIs
Publication statusPublished - 16 Aug 2018

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