Supercooled Silica Research Articles

On the nontrivial wave-vector dependence of the elastic modulus of glasses

Recent theoretical models for the vibrations in glasses assume that the complex elastic modulus depends on frequency but not on the wave vector, $q$. This assumption translates in a simple $q$ dependence of the dynamic structure factor, which can be experimentally tested. Following the suggestion of a recent paper [U. Buchenau, Phys. Rev. E 90, 062319 (2014)], we present here a new analysis, performed in $q$ space, of inelastic x-ray scattering data of supercooled silica. The outcome of the analysis is compared to the more common approach in the frequency domain and indicates that the mentioned theoretical assumption is consistent with the data only below the boson peak frequency. At higher frequencies it gives rise to a breakdown of the classical second moment sum rule. This violation arises from the underlying assumption of the presence of a single excitation in the spectra. A comparison with the vibrational dynamics of $\ensuremath{\alpha}$-cristobalite suggests, on the contrary, that in the terahertz frequency domain the inelastic spectrum of the glass gains contributions from both acousticlike and opticlike modes. A microscopic theory of the vibrations in glasses cannot neglect the medium range order in their structure, which gives rise to dispersion curves within a pseudo-Brillouin zone.

The kinetic fragility of liquids as manifestation of the elastic softening.

We show that the fragility m , the steepness of the viscosity and relaxation time close to the vitrification, increases with the degree of elastic softening, i.e. the decrease of the elastic modulus with increasing temperature, in a universal way. This provides a novel connection between the thermodynamics, via the modulus, and the kinetics. The finding is evidenced by numerical simulations and comparison with the experimental data of glassformers with widely different fragilities (33 ≤ m ≤ 115), leading to a fragility-independent elastic master curve extending over eighteen decades in viscosity and relaxation time. The master curve is accounted for by a cavity model pointing out the roles of both the available free volume and the cage softness. A major implication of our findings is that ultraslow relaxations, hardly characterised experimentally, become predictable by linear elasticity. As an example, the viscosity of supercooled silica is derived over about fifteen decades with no adjustable parameters.

Aging effects in supercooled silica.: A molecular dynamics investigation

Using molecular dynamics simulations we investigate the presence of dynamical heterogeneities in supercooled silica, a ‘strong’ glass former, and the changes as a function of time of these heterogeneities during aging. We compare the radial distribution functions for the 10% most mobile silicon or oxygen atoms with the corresponding mean radial distribution functions. We measure changes of these radial distribution functions and the changes of the non-gaussian parameters with time after a quench. We find that dynamical heterogeneities are present in silica and that they increase during the aging process. We find that the oxygen and silicon atoms show similar heterogeneities but with a differing rate of change during aging.

Instantaneous normal modes analysis of amorphous and supercooled silica

The dynamics of a model for amorphous and supercooled silica (SiO2), a strong glass former, is studied using instantaneous normal mode (INM) analysis. The INM spectra at a variety of temperatures are calculated via molecular dynamics simulation. At temperatures below the glass transition temperature, the dominant contribution to the soft highly anharmonic modes comprising the imaginary frequency region of the INM spectrum are found to correspond to coupled rotations of SiO4 tetrahedral units, consistent with interpretations of neutron scattering experiments [B. B. Buchenau, H. M. Zhou, and N. Nucker, Phys. Rev. Lett. 60, 1318 (1988)] and with previous normal mode analysis of simulation results at T=0 K [S. N. Taraskin and S. R. Elliot, Phys. Rev. B 56, 8623 (1997)].

Generic mechanism for generating a liquid-liquid phase transition.

Recent experimental results indicate that phosphorus--a single-component system--can have a high-density liquid (HDL) and a low-density liquid (LDL) phase. A first-order transition between two liquids of different densities is consistent with experimental data for a variety of materials, including single-component systems such as water, silica and carbon. Molecular dynamics simulations of very specific models for supercooled water, liquid carbon and supercooled silica predict a LDL-HDL critical point, but a coherent and general interpretation of the LDL-HDL transition is lacking. Here we show that the presence of a LDL and a HDL can be directly related to an interaction potential with an attractive part and two characteristic short-range repulsive distances. This kind of interaction is common to other single-component materials in the liquid state (in particular, liquid metals), and such potentials are often used to describe systems that exhibit a density anomaly. However, our results show that the LDL and HDL phases can occur in systems with no density anomaly. Our results therefore present an experimental challenge to uncover a liquid-liquid transition in systems like liquid metals, regardless of the presence of a density anomaly.

The dynamics of supercooled silica: acoustic modes and boson peak

Using molecular dynamics computer simulations we investigate the dynamics of supercooled silica in the frequency range 0.5–20 THz and the wave-vector range 0.13–3.5 Å −1. We find that for small wave-vectors the dispersion relations are in very good agreement with the ones found in experiments. In particular we discuss the wave-vector dependence of the longitudinal and transverse acoustic modes and of the boson peak.

Molecular dynamics simulation of the dynamics of supercooled silica

We present the results of a large scale computer simulation of supercooled silica. We find that at high temperatures the diffusion constants show a non-Arrhenius temperature dependence whereas at low temperature this dependence is also compatible with an Arrhenius law. We demonstrate that at low temperatures the intermediate scattering function shows a two-step relaxation behavior and that it obeys the time temperature superposition principle. We also discuss the wave-vector dependence of the nonergodicity parameter and the time and temperature dependence of the non-Gaussian parameter.

Molecular dynamics simulation of the dynamics of supercooled silica

Molecular dynamics simulation of the dynamics of supercooled silica