Gas-liquid phase separation at zero temperature: mechanical interpretation and implications for gelation

The relation between glasses and gels has been intensely debated for decades; however, the transition between these two phases remains elusive. In this study, we conducted numerical experiments of athermal quasistatic decompression to investigate a gas-liquid phase separation, which is one of the main gel formation processes. A normal mode analysis revealed that the phase separation is signaled by the vanishing of the lowest eigenenergy, similar to plastic events under shear. One primary difference from the shear-induced plasticity is that the vanishing mode experiences a qualitative change in its spatial energy distribution at the phase separation point. These findings enable us to define gelation based on mechanics.Comment: 13 pages, 11 figure

Spatial structure of quasi-localized vibrations in nearly jammed amorphous solids

The low-temperature properties of amorphous solids are widely believed to be controlled by low-frequency quasi-localized modes. What governs their spatial structure and density is however debated. We study these questions numerically in very large systems as the jamming transition is approached and the pressure p vanishes. We find that these modes consist of an unstable core in which particles undergo the buckling motions and decrease the energy, and a stable far-field component which increases the energy and prevents the buckling of the core. The size of the core diverges as $p^{-1/4}$ and its characteristic volume as $p^{-1/2}$ These features are precisely those of the anomalous modes known to cause the Boson peak in the vibrational spectrum of weakly-coordinated materials. From this correspondence we deduce that the density of quasi-localized modes must go as $g_{\mathrm{loc}}(\omega) \sim \omega^4/p^2$ , in agreement with previous observations. Our analysis thus unravels the nature of quasi-localized modes in a class of amorphous materials.Comment: 5 pages, 4 figure

Vibrational density of states of jammed packing: mean-field theory and beyond

Several mean-field theories predict that Hessian matrices of amorphous solids can be written by using the random matrix in the limit of the large spatial dimensions $d\to\infty$. Motivated by these results, we here propose a way to map a Hessian of the amorphous solid to a random matrix. This is possible by determining the coefficients of a random matrix so that the trace of the random matrix coincides with the Hessian of the original system. We compare our result with that of previous numerical simulations of harmonic spheres in several spatial dimensions $d=3$, $5$, and $9$. For small pressure $p\ll 1$ (near jamming), we find a good agreement even in $d=3$, and obtain better agreements in larger $d$, suggesting that the approximation indeed becomes exact in the limit of large spatial dimensions. We also discuss the finite dimensional effects, which are not considered in the mean-field theory and lead to the coexistence of the Debye density of state $D(\omega)\sim \omega^{d-1}$ and the quartic mode $D(\omega)\sim \omega^4$ for small $\omega$.Comment: 6 pages, 2 figure

Spatial structure of unstable normal modes in a glass-forming liquid

The phenomenology of glass-forming liquids is often described in terms of their underlying, high-dimensional potential energy surface. In particular, the statistics of stationary points sampled as a function of temperature provides useful insight into the thermodynamics and dynamics of the system. To make contact with the real space physics, however, analysis of the spatial structure of the normal modes is required. In this work, we numerically study the potential energy surface of a glass-forming ternary mixture. Starting from liquid configurations equilibrated over a broad range of temperatures using a swap Monte Carlo method, we locate the nearby stationary points and investigate the spatial architecture and the energetics of the associated unstable modes. Through this spatially-resolved analysis, originally developed to study local minima, we corroborate recent evidence that the nature of the unstable modes changes from delocalized to localized around the mode-coupling temperature. We find that the displacement amplitudes of the delocalized modes have a slowly decaying far field, whereas the localized modes consist of a core with large displacements and a rapidly decaying far field. The fractal dimension of unstable modes around the mobility edge is equal to 1, consistent with the scaling of the participation ratio. Finally, we find that around and below the mode-coupling temperature the unstable modes are localized around structural defects, characterized by a disordered local structure markedly different from the liquid's locally favored structure. These defects are similar to those associated to quasi-localized vibrations in local minima and are good candidates to predict the emergence of localized excitations at low temperature