Thermodynamic signature of growing amorphous order in glass-forming liquids

By Giulio Biroli, Jean-Philippe Bouchaud, Andrea Cavagna, T. Grigera, P. Verrocchio. 2008

285 citations recorded by the source corpus.

That the dynamical properties of a glass-forming liquid at high temperature are different from behaviour in the supercooled state has already been established. Numerical simulations now suggest that the static length scale over which spatial correlations exist also changes on approaching the glass transition. Supercooled liquids exhibit a pronounced slowdown of their dynamics on cooling1 without showing any obvious structural or thermodynamic changes2. Several theories relate this slowdown to increasing spatial correlations3,4,5,6. However, no sign of this is seen in standard static correlation functions, despite indirect evidence from considering specific heat7 and linear dielectric susceptibility8. Whereas the dynamic correlation function progressively becomes more non-exponential as the temperature is reduced, so far no similar signature has been found in static correlations that can distinguish qualitatively between a high-temperature and a deeply supercooled glass-forming liquid in equilibrium. Here, we show evidence of a qualitative thermodynamic signature that differentiates between the two. We show by numerical simulations with fixed boundary conditions that the influence of the boundary propagates into the bulk over increasing length scales on cooling. With the increase of this static correlation length, the influence of the boundary decays non-exponentially. Such long-range susceptibility to boundary conditions is expected within the random first-order theory4,9,10 (RFOT) of the glass transition. However, a quantitative account of our numerical results requires a generalization of RFOT, taking into account surface tension fluctuations between states.

Subfields: Ceramics and Composites, Condensed Matter Physics, Materials Chemistry

View Paper: https://www.semanticscholar.org/paper/19279eec61a7701a4668590e0e632df288448fb3

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In Ceramics and Composites

In Condensed Matter Physics

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Citations in the corpus

Swift: A language for distributed parallel scripting (2011, methodology): “Glen Hocky of the Reichman Group at Columbia is evaluating a new cavity method [31] for measuring this length scale, where particles are simulated by molecular dynamics or Monte Carlo methods within cavities having amorphous boundary conditions.”
Theoretical perspective on the glass transition and amorphous materials (2010, unknown): “(60) does increase upon supercooling (Biroli et al., 2008).”
The role of local structure in dynamical arrest (2014, background): “It is also possible to define a structural correlation length via a point-to-set, or pinning approach (section IIID) [55].”
Mean-field theory of hard sphere glasses and jamming (2008, background): “However, the study of the latter has very recently become the subject of intense numerical effort (Biroli et al., 2008; Cammarota et al., 2009), which will hopefully lead to a more complete understanding of the properties of glassy states.”
Facets of glass physics (2015, background): “Additionally, researchers are developing novel computational techniques to explore experimentally relevant temperature regimes and provide more direct insight into the validity of mean-field theory in finite dimensions [10].”
Models and Algorithms for the Next Generation of Glass Transition Studies (2017, methodology): “The swap algorithm has since been mostly used in the glass context, for both binary mixtures [39– 42] and for continuously polydisperse systems [43–45].”