Exposing a dynamical signature of the freezing transition through the sound propagation gap

V. A. Martinez, E. Zaccarelli, E. Sanz, C. Valeriani, W. van Megen*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

Abstract

The conventional view of freezing holds that nuclei of the crystal phase form in the metastable fluid through purely stochastic thermal density fluctuations. The possibility of a change in the character of the fluctuations as the freezing point is traversed is beyond the scope of this perspective. Here we show that this perspective may be incomplete by examination of the time autocorrelation function of the longitudinal current, computed by molecular dynamics for the hard-sphere fluid around its freezing point. In the spatial window where sound is overdamped, we identify a change in the long-time decay of the correlation function at the known freezing points of monodisperse and moderately polydisperse systems. The fact that these findings agree with previous experimental studies of colloidal systems in which particle are subject to diffusive dynamics, suggests that the dynamical signature we identify with the freezing transition is a consequence of packing effects alone.

Original languageEnglish
Article number6503
Number of pages8
JournalNature Communications
Volume5
DOIs
Publication statusPublished - Nov 2014

Keywords

  • HARD-SPHERE FLUID
  • NEUTRON-SCATTERING
  • DENSITY-FLUCTUATIONS
  • MONTE-CARLO
  • LIQUID
  • MODES
  • DECAY

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