Deformation of inherent structures to detect long-range correlations in supercooled liquids

Abstract

We propose deformations of inherent structures as a suitable tool for detecting structural changes underlying the onset of cooperativity in supercooled liquids. The non-affine displacement (NAD) field resulting from the applied deformation shows characteristic differences between the high temperature liquid and supercooled state, which are typically observed in dynamic quantities. The average magnitude of the NAD is very sensitive to temperature changes in the supercooled regime and is found to be strongly correlated with the inherent structure energy. In addition, the NAD field is characterized by a correlation length that increases upon lowering the temperature towards the supercooled regime.

Bond orientational order in liquids: Towards a unified description of water-like anomalies, liquid-liquid transition, glass transition, and crystallization

“…So it is natural to expect that inherent structures have a close relation to our glassy structural order. For exam-ple, the similarity between our results for static growing length and those obtained by Mosayebi et al [355] suggests such a relation. There is certainly a connection, but here we mention a few important difference.…”

“…[296] found a diverging static lengthscale by analysing the response of the inherent structure to static perturbation. Similarly, for binary hard and soft sphere mixtures, no local ordering, nor structural lengthscale has been found to accompany the growing dynamical lengthscale [353,306,351,354], but again Mosayebi et al found the opposite for the latter mixture [355]. The presence of a growing static length in Kob-Andersen and repulsive binary mixtures has also been reported by Karmakar and Procaccia [356].…”

The role of local structure in dynamical arrest

“…The discrepancy observed by most between structural and dynamic lengthscales in the T T MCT range is indicative that more is at play than structure, at least in the first few decades of dynamic slowing which are described by mode-coupling theory. However, it has been shown again and again [82,83,86,143,248,260,261,326,327,368,369,394,442,473,488,507,570] that the structure of deeply supercooled liquids is distinct from that of high temperature liquids and that particular locally favoured structures correspond to dynamically slow particles [300,326,327,394,473,507]. Along with others [86], we believe any coincidence in structural and dynamic lengthscales in the dynamical regime accessible to simulation may be obscured by the mode-coupling transition and that to resolve this question deeper supercooling is required.…”

“…However, as discussed in section V C, this simultaneous increase has certainly not universally been found, especially in d = 3. Indeed, while some groups have identified a concurrent increase of structural and dynamic lengthscales [261,300,368,369,442,507], the majority seem to find that the dynamic correlation length as determined by the four-point correlation length ξ 4 increases faster than the static length, sometimes even in the same system [86,138,218,255,256,277,326,416,500].…”

Nonequilibrium Phase Transition in an Atomistic Glassformer: The Connection to Thermodynamics

“…Returning to the idea of a thermodynamic transition, a key aspect is some kind of structural change. While such structural changes appear to be minor when looking at two-point measures like the structure factor, higher-order measures reveal a richer behavior [20][21][22][23][24][25]. In particular, the population of geometric motifs, so-called locally favoured structures (LFS), show a strong temperaturedependence [20].…”