Dielectric Spectroscopy and Ultrasonic Study of Propylene Carbonate under Ultra-high Pressures

TL;DR

This study combines dielectric spectroscopy and ultrasonic measurements to explore the behavior of propylene carbonate under ultra-high pressures, revealing a simple relaxation process and insights into its elastic and molecular properties.

Contribution

It provides the first high-pressure dielectric and ultrasonic data on propylene carbonate, extending the equation of state and analyzing relaxation and elastic properties under extreme conditions.

Findings

Only $oldsymbol{ m f extit{ ext{alpha}}}$-relaxation observed at high pressures.

Elastic moduli and Poisson's ratio measured up to 1.7 GPa.

Pressure affects the correlation between Poisson's ratio and fragility.

Abstract

We present the high pressure dielectric spectroscopy (up to 4.2 GPa) and ultrasonic study (up to 1.7 GPa) of liquid and glassy propylene carbonate (PC). Both of the methods provide complementary pictures of the glass transition in PC under pressure. No other relaxation processes except $\alpha$-relaxation have been found in the studied pressure interval. The propylene carbonate liquid is a glassformer where simple relaxation and the absence of $\beta$-relaxation are registered in the record-breaking ranges of pressures and densities. The equation of state of liquid PC was extended up to 1 GPa from ultrasonic measurements of bulk modulus and is in good accordance with the previous equations developed from volumetric data. We measured the bulk and shear moduli and Poisson's ratio of glassy PC up to 1.7 GPa. Many relaxation and elastic properties of PC can be qualitatively described by the soft-sphere or Lennard-Jones model. However, for the quantitative description of entire set of the experimental data, these models are insufficient. Moreover, the Poisson coefficient value for glassy PC indicates a significant contribution of non-central forces to the intermolecular potential. The well-known correlation between Poisson's ratio and fragility index (obtained from dielectric relaxation) is confirmed for PC at ambient pressure, but it is violated with pressure increase. This indicates that different features of the potential energy landscape are responsible for the evolution of dielectric response and elasticity with pressure increase.