Structural, mechanical, and vibrational properties of particulate physical gels

TL;DR

This study uses molecular dynamics simulations to analyze particulate physical gels, revealing their unique structural, mechanical, and vibrational properties and how these differ from glasses, highlighting their multiscale nature.

Contribution

It provides a comprehensive understanding of the structural, mechanical, and vibrational properties of Lennard-Jones gels, a model for particulate physical gels, which was previously limited.

Findings

Gels have sparse, heterogeneous structures with size scale $\xi_s$ increasing as density decreases.

Gels are extremely soft with shear and bulk moduli much smaller than glasses.

Vibrational density of states shows a plateau with a characteristic onset frequency $\omega_\ast$.

Abstract

Our lives are surrounded by a rich assortment of disordered materials. In particular, glasses are well known as dense, amorphous materials, whereas gels exist in low-density, disordered states. Recent progress has provided a significant step forward in understanding the material properties of glasses, such as mechanical, vibrational, and transport properties. In contrast, our understanding of particulate physical gels is still highly limited. Here, using molecular dynamics simulations, we study a simple model of particulate physical gels, the Lennard-Jones (LJ) gels, and provide a comprehensive understanding of their structural, mechanical, and vibrational properties, all of which are markedly different from those of glasses. First, the LJ gels show sparse, heterogeneous structures, and the length scale $\xi_s$ of the structures grows as the density is lowered. Second, the gels are extremely soft, with both shear $G$ and bulk $K$ moduli being orders of magnitude smaller than those of glasses. Third, many low-frequency vibrational modes are excited, which form a characteristic plateau with the onset frequency $\omega_\ast$ in the vibrational density of states. Structural, mechanical, and vibrational properties, characterized by $\xi_s$, $G$, $K$, and $\omega_\ast$, respectively, show power-law scaling behaviors with the density, which establishes a close relationship between them. Throughout the present work, we reveal that gels are multiscale, solid-state materials: (i) homogeneous elastic bodies at long lengths, (ii) heterogeneous elastic bodies with fractal structures at intermediate lengths, and (iii) amorphous structural bodies at short lengths.