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Title: Signature of collective elastic glass physics in surface-induced long-range tails in dynamical gradients
Understanding the underlying nature of dynamical correlations believed to drive the bulk glass transition is a long-standing problem. Here we show that the form of spatial gradients of the glass transition temperature and structural relaxation time near an interface indeed provide signatures of the nature of relaxation in bulk glass forming liquids. We report results of long-time, large-system molecular dynamics simulations of thick glass-forming polymer films with one vapor interface, supported on a dynamically neutral substrate. We find that gradients in the glass transition temperature and logarithm of the structural relaxation time nucleated at a vapor interface exhibit two distinct regimes: a medium-ranged, large amplitude exponential gradient, followed by a long-range slowly decaying tail that can be described by an inverse power law. This behavior disagrees with multiple proposed theories of glassy dynamics but is predicted by the Elastically Collective Nonlinear Langevin Equation theory as a consequence of two coupled mechanisms: a medium-ranged interface-nucleated gradient of surface modified local caging constraints, and an interfacial truncation of a long-ranged collective elastic field. These findings support a coupled spatially local-nonlocal mechanism of activated glassy relaxation and kinetic vitrification.in both the isotropic bulk and in broken symmetry films.  more » « less
Award ID(s):
1849594
PAR ID:
10471339
Author(s) / Creator(s):
; ; ;
Publisher / Repository:
Nature Porfolio
Date Published:
Journal Name:
Nature Physics
Volume:
19
Issue:
6
ISSN:
1745-2473
Page Range / eLocation ID:
800 to 806
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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