arXiv subjects

Asaph Widmer-Cooper

Publications and source records attributed to Asaph Widmer-Cooper.

24 records · Page 2Linked to original sources

arXiv2009

Localised soft modes and the supercooled liquid's irreversible passage through its configuration space

Using computer simulations, we show that the localized low frequency normal modes of a configuration in a supercooled liquid are strongly correlated with the irreversible structural reorganization of the particles within that configuration. Establishing this correlation constitutes the identification of the aspect of a configuration that determines the heterogeneity of the subsequent motion. We demonstrate that the spatial distribution of the summation over the soft local modes can persist in spite of particle reorganization that produces significant changes in individual modes. Along with spatial localization, the persistent influence of soft modes in particle relaxation results in anisotropy in the displacements of mobile particles over the timescale referred to as beta relaxation.

cond-mat.soft↗

arXiv2009

On the relationship between structure and dynamics in a supercooled liquid

We present the dynamic propensity distribution as an explicit measure of the degree to which the dynamics in a liquid over the time scale of structural relaxation is determined by the initial configuration. We then examine, for a binary mixture of soft discs in two dimensions, the correlation between the spatial distribution of propensity and that of two localmeasures of configuration structure: the local composition and local free volume. While the small particles dominate the high propensity population,we find no strong correlation between either the local composition or the local free volume and the propensity. It is argued that this is a generic failure of purely local structural measures to capture the inherently non-local character of collective behaviour.

cond-mat.stat-mech↗

arXiv2009

On the Study of Collective Dynamics in Supercooled Liquids through the Statistics of the Iso-Configurational Ensemble

The use of the isoconfigurational ensemble to explore structure-dynamic correlations in supercooled liquids is examined. The statistical error of the dynamic propensity and its spatial distribution are determined. The authors present the spatial distribution of the particle non-Gaussian parameter as a measure of the intermittency with which particles exhibit their propensity for motion. The ensemble average of the direction of particle motion is introduced to establish the anisotropy of the dynamic propensity.

cond-mat.stat-mech↗

arXiv2009

Irreversible reorganization in a supercooled liquid originates from localised soft modes

The transition of a fluid to a rigid glass upon cooling is a common route of transformation from liquid to solid that embodies the most poorly understood features of both phases1,2,3. From the liquid perspective, the puzzle is to understand stress relaxation in the disordered state. From the perspective of solids, the challenge is to extend our description of structure and its mechanical consequences to materials without long range order. Using computer simulations, we show that the localized low frequency normal modes of a configuration in a supercooled liquid are causally correlated to the irreversible structural reorganization of the particles within that configuration. We also demonstrate that the spatial distribution of these soft local modes can persist in spite of significant particle reorganization. The consequence of these two results is that it is now feasible to construct a theory of relaxation length scales in glass-forming liquids without recourse to dynamics and to explicitly relate molecular properties to their collective relaxation.

cond-mat.soft↗

arXiv2005

Predicting the long time dynamic heterogeneity in a supercooled liquid on the basis of short time heterogeneities

We report that the local Debye-Waller factor in a simulated 2D glass-forming mixture exhibits significant spatial heterogeneities and that these short time fluctuations provide an excellent predictor of the spatial distribution of the long time dynamic propensities [Phys.Rev.Lett. 93, 135701 (2004)]. In contrast, the potential energy per particle of the inherent structure does not correlate well with the spatially distributed dynamics.

cond-mat.stat-mech↗

arXiv2005

Free Volume cannot Explain the Spatial Heterogeneity of Debye-Waller factors in a Glass-Forming Binary Alloy

We examine the relation between the free volume per particle and the variance of the particle position, equivalent to a local Debye-Waller (DW) factor for a 2D glass-forming alloy using molecular dynamics simulations. We find that the latter quantity exhibits significant spatial heterogeneity despite involving trajectories two orders of magnitude shorter than those typically used to measure such heterogeneities. We find that the free volume exhibits no significant spatial correlation with the local DW factor. We conclude that the spatial variation in local free volume is not the cause of the short time dynamic heterogeneity.

cond-mat.dis-nn↗