Excitations are localized and relaxation is hierarchical in glass-forming liquids

ORAL

Abstract

For several atomistic models of glass formers, at conditions below their glassy dynamics onset temperatures, $T_{\mathrm{o}}$, we use importance sampling of trajectory space to study the structure, statistics and dynamics of excitations responsible for structural relaxation. Excitations are detected in terms of persistent particle displacements of length $a$. At supercooled conditions, for $a$ of the order of or smaller than a particle diameter, we find that excitations are associated with correlated particle motions that are sparse and localized, occupying a volume with an average radius that is temperature independent and no larger than a few particle diameters. We show that the statistics and dynamics of these excitations are facilitated and hierarchical. Excitation energy scales grow logarithmically with $a$. Excitations at one point in space facilitate the birth and death of excitations at neighboring locations, and space-time excitation structures are microcosms of heterogeneous dynamics at larger scales. This nature of dynamics becomes increasingly dominant as temperature $T$ is lowered. We show that slowing of dynamics upon decreasing temperature below $T_{\mathrm{o}}$ is the result of a decreasing concentration of excitations and concomitant growing hierarchical leng

Authors

  • Aaron Keys

    • University of Michigan Chemical Engineering Dept
    • Lawrence Berkeley National Laboratory
  • Lester Hedges

    • Lawrence Berkeley National Laboratory
  • Juan Garrahan

    • School of Physics and Astronomy, University of Nottingham, Nottingham NG7 2RD, UK
    • University of Nottingham
  • Sharon Glotzer

    • University of Michigan
    • Department of Chemical Engineering, University of Michigan, Ann Arbor, MI
    • University of Michigan Chemical Engineering Dept
    • University of Michigan, Dept. of Chemical Engineering
    • Department of Chemical Engineering, University of Michigan
  • David Chandler

    • University of California, Berkeley