Predicting the Density-scaling Exponent of a Glass-forming Liquid from Prigogine-Defay Ratio Measurements

Understanding the origin of the dramatic temperature and density dependence of the relaxation time of glass-forming liquids is a fundamental challenge in glass science. The recently established density-scaling relation quantifies the relative importance of temperature and density for the relaxation time in terms of a material-dependent exponent. We show that this exponent for approximate single-parameter liquids can be calculated from thermoviscoelastic linear-response data at a single state point, for instance an ambient-pressure state point. This prediction is confirmed for the van der Waals liquid tetramethyl-tetraphenyl-trisiloxane. Consistent with this, a compilation of literature data for the Prigogine-Defay ratio shows that van derWaals liquids and polymers are approximate single-parameter systems, whereas associated and network-forming liquids are not.
Published in Nature Physics, PUBLISHED ONLINE: 3 JULY 2011,Government or Federal Purpose Rights License.. The original document contains color images.