Vibrational lifetimes and viscoelastic properties of ultrastable glasses

Abstract

Amorphous solids are viscoelastic. They dissipate energy when deformed at finite rate and finite temperature. We here use analytic theory and molecular simulations to demonstrate that linear viscoelastic dissipation can be directly related to the static and dynamic properties of the fundamental vibrational excitations of an amorphous system. We study ultrastable glasses that do not age, i.e., that remain in stable minima of the potential energy surface at finite temperature. Our simulations show four types of vibrational modes, which differ in spatial localization, similarity to plane waves and vibrational lifetimes. At frequencies below the Boson peak, the viscoelastic response can be split into contributions from plane-wave and quasilocalized modes. We derive a parameter-free expression for the viscoelastic storage and loss moduli for both of these modes. Our results show that the dynamics of microscopic dissipation, in particular the lifetimes of the modes, determine the viscoelastic response only at high frequency. Quasilocalized modes dominate the linear viscoelastic response at intermediate frequencies below the Boson peak.