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
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Authors
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Aaron Keys
University of Michigan Chemical Engineering Dept, Lawrence Berkeley National Laboratory
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Lester Hedges
Lawrence Berkeley National Laboratory
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Juan Garrahan
School of Physics and Astronomy, University of Nottingham, Nottingham NG7 2RD, UK, University of Nottingham
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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
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David Chandler
University of California, Berkeley