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Title: Relationship between local structure and relaxation in out-of-equilibrium glassy systems

Abstract

The dynamical glass transition is typically taken to be the temperature at which a glassy liquid is no longer able to equilibrate on experimental timescales. Consequently, the physical properties of these systems just above or below the dynamical glass transition, such as viscosity, can change by many orders of magnitude over long periods of time following external perturbation. During this progress toward equilibrium, glassy systems exhibit a history dependence that has complicated their study. In previous work, we bridged the gap between structure and dynamics in glassy liquids above their dynamical glass transition temperatures by introducing a scalar field called “softness,” a quantity obtained using machine-learning methods. Softness is designed to capture the hidden patterns in relative particle positions that correlate strongly with dynamical rearrangements of particle positions. Here we show that the out-of-equilibrium behavior of a model glass-forming system can be understood in terms of softness. We first demonstrate that the evolution of behavior following a temperature quench is a primarily structural phenomenon: The structure changes considerably, but the relationship between structure and dynamics remains invariant. We then show that the relaxation time can be robustly computed from structure as quantified by softness, with the same relation holding bothmore » in equilibrium and as the system ages. Together, these results show that the history dependence of the relaxation time in glasses requires knowledge only of the softness in addition to the usual state variables.« less

Authors:
ORCiD logo [1];  [2];  [2];  [3]
+ Show Author Affiliations
  1. Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Physics and Astronomy; Harvard Univ., Boston, MA (United States). School of Engineering and Applied Sciences
  2. Harvard Univ., Boston, MA (United States). School of Engineering and Applied Sciences
  3. Univ. of Pennsylvania, Philadelphia, PA (United States). Dept. of Physics and Astronomy
Publication Date:
Research Org.:
Univ. of Pennsylvania, Philadelphia, PA (United States); Harvard Univ., Cambridge, MA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; Simons Foundation
OSTI Identifier:
1337592
Alternate Identifier(s):
OSTI ID: 1430119
Grant/Contract Number:  
FG02‐05ER46199; FG02-05ER46199
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 114 Journal Issue: 2; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 97 MATHEMATICS AND COMPUTING; glasses; aging; structure; machine learning

Citation Formats

Schoenholz, Samuel S., Cubuk, Ekin D., Kaxiras, Efthimios, and Liu, Andrea J. Relationship between local structure and relaxation in out-of-equilibrium glassy systems. United States: N. p., 2016. Web. doi:10.1073/pnas.1610204114.
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Schoenholz, Samuel S., Cubuk, Ekin D., Kaxiras, Efthimios, & Liu, Andrea J. Relationship between local structure and relaxation in out-of-equilibrium glassy systems. United States. https://doi.org/10.1073/pnas.1610204114
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Schoenholz, Samuel S., Cubuk, Ekin D., Kaxiras, Efthimios, and Liu, Andrea J. Tue . "Relationship between local structure and relaxation in out-of-equilibrium glassy systems". United States. https://doi.org/10.1073/pnas.1610204114.
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@article{osti_1337592,
title = {Relationship between local structure and relaxation in out-of-equilibrium glassy systems},
author = {Schoenholz, Samuel S. and Cubuk, Ekin D. and Kaxiras, Efthimios and Liu, Andrea J.},
abstractNote = {The dynamical glass transition is typically taken to be the temperature at which a glassy liquid is no longer able to equilibrate on experimental timescales. Consequently, the physical properties of these systems just above or below the dynamical glass transition, such as viscosity, can change by many orders of magnitude over long periods of time following external perturbation. During this progress toward equilibrium, glassy systems exhibit a history dependence that has complicated their study. In previous work, we bridged the gap between structure and dynamics in glassy liquids above their dynamical glass transition temperatures by introducing a scalar field called “softness,” a quantity obtained using machine-learning methods. Softness is designed to capture the hidden patterns in relative particle positions that correlate strongly with dynamical rearrangements of particle positions. Here we show that the out-of-equilibrium behavior of a model glass-forming system can be understood in terms of softness. We first demonstrate that the evolution of behavior following a temperature quench is a primarily structural phenomenon: The structure changes considerably, but the relationship between structure and dynamics remains invariant. We then show that the relaxation time can be robustly computed from structure as quantified by softness, with the same relation holding both in equilibrium and as the system ages. Together, these results show that the history dependence of the relaxation time in glasses requires knowledge only of the softness in addition to the usual state variables.},
doi = {10.1073/pnas.1610204114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 2,
volume = 114,
place = {United States},
year = {Tue Dec 27 00:00:00 EST 2016},
month = {Tue Dec 27 00:00:00 EST 2016}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1073/pnas.1610204114
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