Dimensional study of the caging order parameter at the glass transition

Proc Natl Acad Sci U S A. 2012 Aug 28;109(35):13939-43. doi: 10.1073/pnas.1211825109. Epub 2012 Aug 13.

Abstract

The glass problem is notoriously hard and controversial. Even at the mean-field level, little is agreed upon regarding why a fluid becomes sluggish while exhibiting but unremarkable structural changes. It is clear, however, that the process involves self-caging, which provides an order parameter for the transition. It is also broadly assumed that this cage should have a gaussian shape in the mean-field limit. Here we show that this ansatz does not hold. By performing simulations as a function of spatial dimension d, we find the cage to keep a nontrivial form. Quantitative mean-field descriptions of the glass transition, such as mode-coupling theory, density functional theory, and replica theory, all miss this crucial element. Although the mean-field random first-order transition scenario of the glass transition is qualitatively supported here and non-mean-field corrections are found to remain small on decreasing d, reconsideration of its implementation is needed for it to result in a coherent description of experimental observations.

Publication types

  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Cold Temperature
  • Glass / chemistry*
  • Hydrodynamics*
  • Models, Chemical*
  • Molecular Dynamics Simulation*
  • Normal Distribution
  • Phase Transition*