Dynamic Entropy as a Measure of Caging and Persisent Particle Motion in Supercooled Liquids

Published

November 1, 1999

Author(s)

P Allegrini, Jack F. Douglas, S C. Glotzer

Abstract

The length-scale dependence of the dynamic entropy is studied in a molecular dynamics simulation of a binary Lennard-Jones liquid above the mode-coupling critical temperature T_c. A number of methods exist for estimating the entropy of dynamical systems and we utilize an approximation based on calculating the mean first-passage time (MFPT) for particle displacement because of its tractability and its accessibility in real and simulation measurements. The MFPT dynamic entropy S(ε) is defined to equal the inverse of the average first-passage time for a particle to exit a sphere of radius ε. This measure of the degree of chaotic motion allows us to identify characteristic time and space scales and to quantify the increasingly correlated particle motion and intermittency occurring in supercooled liquids. In particular, we identify a cage size defining the scale at which the particles are transiently localized, and we observe persistent particle motion at intermediate length scales beyond the scale where caging occurs. Furthermore, we find that the dynamic entropy at the scale of one interparticle spacing extrapolates to zero as the mode-coupling temperature T_c is approached.

Citation

Physical Review E (Statistical, Nonlinear, and Soft Matter Physics)

Volume

60

Issue

No. 5

Pub Type

Journals

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Keywords

computer simulations, glasses, supercooled liquids, transport properties

Citation

Allegrini, P. , Douglas, J. and Glotzer, S. (1999), Dynamic Entropy as a Measure of Caging and Persisent Particle Motion in Supercooled Liquids, Physical Review E (Statistical, Nonlinear, and Soft Matter Physics), [online], https://tsapps.nist.gov/publication/get_pdf.cfm?pub_id=851557 (Accessed October 17, 2025)