Anomalous behavior and structure of a liquid of particles interacting through the harmonic-repulsive pair potential near the crystallization transition

Abstract

A characteristic property of many soft matter systems is an ultrasoft effective interaction between their structural units. This softness often leads to complex behavior. In particular, ultrasoft systems under pressure demonstrate polymorphism of complex crystal and quasicrystal structures. Therefore, it is of interest to investigate how different can be the structure of the fluid state in such systems at different pressures. Here we address this issue for the model liquid composed of particles interacting through the harmonic-repulsive pair potential. This system can form different crystal structures as the liquid is cooled. We find that, at certain pressures, the liquid exhibits unusual properties, such as the negative thermal expansion coefficient. Besides, the volume and the potential energy of the system can increase during crystallization. At certain pressures, the system demonstrates high stability against crystallization and it is hardly possible to crystallize it on the timescales of the simulations. To address the liquid's structure at high pressures, we consider the scaled pair distribution function (PDF) and the bond-orientational order (BOO) parameters. The marked change happening with the PDF, as pressure increases, is the splitting of the first peak which is caused by the appearance of non-negligible interaction with the second neighbors and the following rearrangement of the structure. Our findings suggest that non-trivial effects, usually explained by different interactions at different spatial scales, can be observed also in one-component systems with simple one-length-scale ultrasoft repulsive interactions.

arXiv comment18 pages, 17 figures

References in corpus (19)

• Dynamics on the Way to Forming Glass: Bubbles in Space-time
• The role of local structure in dynamical arrest
• Can Polymer Coils be modeled as "Soft Colloids"?
• Exact Criterion for Determining Clustering vs. Reentrant Melting Behavior for Bounded Interaction Potentials
• The glass transition of soft colloids
• Water-Like Anomalies for Core-Softened Models of Fluids: Two-Dimensional Systems
• Microscopic theory of the jamming transition of harmonic spheres
• Anomalous structure factor of dense star polymer solutions
• Exotic fluids and crystals of soft polymeric colloids
• Superfragile glassy dynamics of onecomponent system with isotropic potential: competition of diffusion and frustration
• Anomalous phase behavior of a soft-repulsive potential with a strictly monotonic force
• Cooling rate dependence of simulated $\mathrm{C}{\mathrm{u}}_{64.5}\mathrm{Z}{\mathrm{r}}_{35.5}$ metallic glass structure
• The zero-temperature phase diagram of soft-repulsive particle fluids
• Two stage order-disorder transformation in simple monatomic supercritical fluid: superstable tetrahedral local order
• Anomalous melting behavior under extreme conditions: hard matter turning "soft"
• Glass Formation and Crystallization of a Simple Monatomic Liquid
• Polymorph selection during crystallization of a model colloidal fluid with a free energy landscape containing a metastable solid
• Crystalline structures of particles interacting through the harmonic-repulsive pair potential
• Green-Kubo stress correlation function at the atomic scale and a long-range bond-orientational ordering in a model liquid