Role of structural relaxations and vibrational excitations in the high-frequency dynamics of liquids and glasses

TL;DR

This paper uses mode-coupling theory to analyze high-frequency dynamics in liquids and glasses, explaining anomalous sound velocity dispersion and the boson peak through structural relaxations and vibrational excitations, with predictions for negative dispersion.

Contribution

It provides a systematic theoretical explanation for anomalous dispersion phenomena in liquids and glasses, linking them to vibrational modes and structural relaxations, and predicts new observable effects.

Findings

Explanation of anomalous sound velocity dispersion across temperature ranges.

Identification of the boson peak as a low-frequency excitation (AOP).

Prediction of negative dispersion when vibrational dynamics dominate.

Abstract

We present theoretical investigation on the high-frequency collective dynamics in liquids and glasses at microscopic length scales and terahertz frequency region based on the mode-coupling theory for ideal liquid-glass transition. We focus on recently investigated issues from inelastic-X-ray-scattering and computer-simulation studies for dynamic structure factors and longitudinal and transversal current spectra: the anomalous dispersion of the high-frequency sound velocity and the nature of the low-frequency excitation called the boson peak. It will be discussed how the sound mode interferes with other low-lying modes present in the system. Thereby, we provide a systematic explanation of the anomalous sound-velocity dispersion in systems -- ranging from high temperature liquid down to deep inside the glass state -- in terms of the contributions from the structural-relaxation processes and from vibrational excitations called the anomalous-oscillation peak (AOP). A possibility of observing negative dispersion -- the {\em decrease} of the sound velocity upon increase of the wave number -- is argued when the sound-velocity dispersion is dominated by the contribution from the vibrational dynamics. We also show that the low-frequency excitation, observable in both of the glass-state longitudinal and transversal current spectra at the same resonance frequency, is the manifestation of the AOP. As a consequence of the presence of the AOP in the transversal current spectra, it is predicted that the transversal sound velocity also exhibits the anomalous dispersion. These results of the theory are demonstrated for a model of the Lennard-Jones system.