Molecular dynamics study of one-component soft-core system: thermodynamic properties in the supercooled liquid and glassy states.

Abstract

Molecular dynamics simulations were performed to study the thermal properties of a supercooled liquid near the glass transition regime and of glasses in a one-component soft-core system with the pair potential φn(r) = ɛ(σ/r)(n), in which n = 12. The results are examined along a phase diagram, in which the compressibility factor defined by [Formula: see text] is plotted against the reduced density ρ* = ρ(ɛ/kBT)(3/n) (or the reduced temperature T* = ρ*(-n/3)). Similarly, a time-dependent dynamical compressibility factor can be plotted against the time-dependent reduced density [Formula: see text] (or the reduced time-dependent temperature). Analytical expressions of the specific heats CV and CP and of the entropy, S, were obtained as a function of [Formula: see text] or of the scaled potential U*. Even for a rapid cooling process, the CV values are found to be affected by non-equilibrium relaxations in the [Formula: see text] region, where [Formula: see text] is the given initial value of [Formula: see text]. The problem of the Kauzmann paradox is discussed using these expressions. The fluctuation of the time-dependent temperature, Tt*, which determines CV, is characterized by the spectra that are obtained by multitaper methods. The thermal fluctuation along the non-equilibrium relaxation under NVE conditions was also examined.