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Title: Activated dynamics in dense fluids of attractive nonspherical particles. I. Kinetic crossover, dynamic free energies, and the physical nature of glasses and gels

Abstract

We apply the center-of-mass versions of naïve mode coupling theory and nonlinear Langevin equation theory to study how short-range attractive interactions modify the onset of localization, activated single-particle dynamics, and the physical nature of the transiently arrested state of a variety of dense nonspherical particle fluids (and the spherical analog) as a function of volume fraction and attraction strength. The form of the dynamic crossover boundary depends on particle shape, but the reentrant glass-fluid-gel phenomenon and the repulsive glass-to-attractive glass crossover always occur. Diverse functional forms of the dynamic free energy are found for all shapes including glasslike, gel-like, a glass-gel form defined by the coexistence of two localization minima and two activation barriers, and a “mixed” attractive glass characterized by a single, very short localization length but an activation barrier located at a large displacement as in repulsive-force caged glasses. For the latter state, particle trajectories are expected to be of a two-step activated form and can be accessed at high attraction strength by increasing volume fraction, or by increasing attraction strength at fixed high enough volume fraction. A new classification scheme for slow dynamics of fluids of dense attractive particles is proposed based on specification of both themore » nature of the localized state and the particle displacements required to restore ergodicity via activated barrier hopping. Here, the proposed physical picture appears to be in qualitative agreement with recent computer simulations and colloid experiments.« less

Authors:
 [1];  [2]
+ Show Author Affiliations
  1. Univ. of Illinois, Urbana, IL (United States); Indian Inst. of Technology, Gandhinagar (India)
  2. Univ. of Illinois, Urbana, IL (United States)
Publication Date:
Research Org.:
Univ. of Illinois at Urbana-Champaign, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1875065
Grant/Contract Number:  
FG02-07ER46471
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics
Additional Journal Information:
Journal Volume: 83; Journal Issue: 4; Journal ID: ISSN 1539-3755
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

Citation Formats

Tripathy, Mukta, and Schweizer, Kenneth S. Activated dynamics in dense fluids of attractive nonspherical particles. I. Kinetic crossover, dynamic free energies, and the physical nature of glasses and gels. United States: N. p., 2011. Web. doi:10.1103/physreve.83.041406.
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Tripathy, Mukta, & Schweizer, Kenneth S. Activated dynamics in dense fluids of attractive nonspherical particles. I. Kinetic crossover, dynamic free energies, and the physical nature of glasses and gels. United States. https://doi.org/10.1103/physreve.83.041406
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Tripathy, Mukta, and Schweizer, Kenneth S. Mon . "Activated dynamics in dense fluids of attractive nonspherical particles. I. Kinetic crossover, dynamic free energies, and the physical nature of glasses and gels". United States. https://doi.org/10.1103/physreve.83.041406. https://www.osti.gov/servlets/purl/1875065.
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@article{osti_1875065,
title = {Activated dynamics in dense fluids of attractive nonspherical particles. I. Kinetic crossover, dynamic free energies, and the physical nature of glasses and gels},
author = {Tripathy, Mukta and Schweizer, Kenneth S.},
abstractNote = {We apply the center-of-mass versions of naïve mode coupling theory and nonlinear Langevin equation theory to study how short-range attractive interactions modify the onset of localization, activated single-particle dynamics, and the physical nature of the transiently arrested state of a variety of dense nonspherical particle fluids (and the spherical analog) as a function of volume fraction and attraction strength. The form of the dynamic crossover boundary depends on particle shape, but the reentrant glass-fluid-gel phenomenon and the repulsive glass-to-attractive glass crossover always occur. Diverse functional forms of the dynamic free energy are found for all shapes including glasslike, gel-like, a glass-gel form defined by the coexistence of two localization minima and two activation barriers, and a “mixed” attractive glass characterized by a single, very short localization length but an activation barrier located at a large displacement as in repulsive-force caged glasses. For the latter state, particle trajectories are expected to be of a two-step activated form and can be accessed at high attraction strength by increasing volume fraction, or by increasing attraction strength at fixed high enough volume fraction. A new classification scheme for slow dynamics of fluids of dense attractive particles is proposed based on specification of both the nature of the localized state and the particle displacements required to restore ergodicity via activated barrier hopping. Here, the proposed physical picture appears to be in qualitative agreement with recent computer simulations and colloid experiments.},
doi = {10.1103/physreve.83.041406},
journal = {Physical Review. E, Statistical, Nonlinear, and Soft Matter Physics},
number = 4,
volume = 83,
place = {United States},
year = {Mon Apr 18 00:00:00 EDT 2011},
month = {Mon Apr 18 00:00:00 EDT 2011}
}
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https://doi.org/10.1103/physreve.83.041406
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    Monte Carlo simulation of cylinders with short-range attractions
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