Microscopic origin of excess wings in relaxation spectra of supercooled liquids

Abstract

Glass formation is encountered in diverse materials. Experiments have revealed that dynamic relaxation spectra of supercooled liquids generically become asymmetric near the glass transition temperature, $T_g$, where an extended power law emerges at high frequencies. The microscopic origin of this "wing" remains unknown, and was so far inaccessible to simulations. Here, we develop a novel computational approach and study the equilibrium dynamics of model supercooled liquids near $T_g$. We demonstrate the emergence of a power law wing in numerical spectra, which originates from relaxation at rare, localised regions over broadly-distributed timescales. We rationalise the asymmetric shape of relaxation spectra by constructing an empirical model associating heterogeneous activated dynamics with dynamic facilitation, which are the two minimal physical ingredients revealed by our simulations. Our work offers a glimpse of the molecular motion responsible for glass formation at relevant experimental conditions.

5 pages, 4 figures, supplementary materials

References in corpus (5)

• Theoretical perspective on the glass transition and amorphous materials
• Glassy Aging Dynamics
• Nonlinear dielectric response at the excess wing of glass-forming liquids
• How to "measure" a structural relaxation time that is too long to be measured?
• Excess wings and asymmetric relaxation spectra in a facilitated trap model

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