Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 115, Issue 1, Pages 87-92Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1711655115
Keywords
sheared fluids; structural entropy; glass transition; slow dynamics; shear thinning
Categories
Funding
- Japan Society of the Promotion of Science [25000002]
- Grants-in-Aid for Scientific Research [25000002] Funding Source: KAKEN
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Glass-forming liquids subjected to sufficiently strong shear universally exhibit striking nonlinear behavior; for example, a powerlaw decrease of the viscosity with increasing shear rate. This phenomenon has attracted considerable attention over the years from both fundamental and applicational viewpoints. However, the out-of-equilibrium and nonlinear nature of sheared fluids have made theoretical understanding of this phenomenon very challenging and thus slower to progress. We find here that the structural relaxation time as a function of the two-body excess entropy, calculated for the extensional axis of the shear flow, collapses onto the corresponding equilibrium curve for a wide range of pair potentials ranging from harsh repulsive to soft and finite. This two-body excess entropy collapse provides a powerful approach to predicting the dynamics of nonequilibrium liquids from their equilibrium counterparts. Furthermore, the two-body excess entropy scaling suggests that sheared dynamics is controlled purely by the liquid structure captured in the form of the two-body excess entropy along the extensional direction, shedding light on the perplexing mechanism behind shear thinning.
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