We present molecular simulation data for viscosity, self-diffusivity, and the local structural ordering of (i) a hard-sphere fluid and (ii) a square-well fluid with short-range attractions. The latter fluid exhibits a region of dynamic anomalies in its phase diagram, where its mobility increases upon isochoric cooling, which is found to be a subset of a larger region of structural anomalies, in which its pair correlations strengthen upon isochoric heating. This “cascade of anomalies” qualitatively resembles that found in recent simulations of liquid water. The results for the hard-sphere and square-well systems also show that the breakdown of the Stokes–Einstein relation upon supercooling occurs for conditions where viscosity and self-diffusivity develop different couplings to the degree of pairwise structural ordering of the liquid. We discuss how these couplings reflect dynamic heterogeneities. Finally, we note that the simulation data suggest how repulsive and attractive glasses may generally be characterized by two distinct levels of short-range structural order.
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28 July 2007
Research Article|
July 23 2007
How short-range attractions impact the structural order, self-diffusivity, and viscosity of a fluid
William P. Krekelberg;
William P. Krekelberg
a)
Department of Chemical Engineering,
University of Texas at Austin
, Austin, Texas 78712, USA
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Jeetain Mittal;
Jeetain Mittal
b)
Laboratory of Chemical Physics, NIDDK,
National Institutes of Health
, Bethesda, Maryland 20892-0520, USA
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Venkat Ganesan;
Venkat Ganesan
c)
Department of Chemical Engineering and Institute for Theoretical Chemistry,
University of Texas at Austin
, Austin, Texas 78712, USA
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Thomas M. Truskett
Thomas M. Truskett
d)
Department of Chemical Engineering and Institute for Theoretical Chemistry,
University of Texas at Austin
, Austin, Texas 78712, USA
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a)
Electronic mail: krekel@che.utexas.edu
b)
Electronic mail: jeetain@helix.nih.gov
c)
Electronic mail: venkat@che.utexas.edu
d)
Author to whom correspondence should be addressed. Electronic mail: truskett@che.utexas.edu
J. Chem. Phys. 127, 044502 (2007)
Article history
Received:
May 02 2007
Accepted:
June 06 2007
Citation
William P. Krekelberg, Jeetain Mittal, Venkat Ganesan, Thomas M. Truskett; How short-range attractions impact the structural order, self-diffusivity, and viscosity of a fluid. J. Chem. Phys. 28 July 2007; 127 (4): 044502. https://doi.org/10.1063/1.2753154
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