Decoupling between thermodynamics and dynamics during rejuvenation in colloidal glasses

Abstract

We rejuvenate well-aged quasi-2D binary colloidal glasses by thermal cycling, and systematically measure both the statistical responses and particle-level structural evolutions during rejuvenation. While the moduli and boson peak are continuously rejuvenated with increasing number of cycles, the mean square displacement (MSD) fluctuates significantly between different groups of thermal cycles. The decoupling between the thermodynamical and dynamical evolutions suggests different microscopic origins for different bulk properties of glasses. We find that a small fraction of structural rearrangements triggered by thermal cycling could alter the whole elastic continuum and lead to the significant thermodynamic rejuvenation, while localized defects could be activated and deactivated at the positions close to the rearrangements with significantly high mobility change and hence result in the fluctuated dynamics even with only about 10% of particles as fast regions. Our results offer a comprehensive picture for the microscopic mechanisms underlying bulk glass rejuvenation, which could be readily used to refine glass properties or to formulate further statistical theories in glassy systems.

Preface: Special issue ‘Unifying Concepts in Glass Physics VII’

“…Other topics in supercooled liquids approaching their glass transition addressed here include density fluctuations, which are often overlooked in glassforming systems [11], Stokes-Einstein relations [12], mean-field theories [13] and configuration-tree theory [14]. Far-from equilibrium phenomena tackled in this special issue range from aging and rejuvenation in the novel context of colloidal experiments [15] to strain fluctuations [16].…”