Equilibrium ultrastable glasses produced by random pinning

Hocky, Glen M.; Reichman, David R.; Berthier, Ludovic

doi:10.1063/1.4903200

Title: Equilibrium ultrastable glasses produced by random pinning

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Abstract

Ultrastable glasses have risen to prominence due to their potentially useful material properties and the tantalizing possibility of a general method of preparation via vapor deposition. Despite the importance of this novel class of amorphous materials, numerical studies have been scarce because achieving ultrastability in atomistic simulations is an enormous challenge. Here, we bypass this difficulty and establish that randomly pinning the position of a small fraction of particles inside an equilibrated supercooled liquid generates ultrastable configurations at essentially no numerical cost, while avoiding undesired structural changes due to the preparation protocol. Building on the analogy with vapor-deposited ultrastable glasses, we study the melting kinetics of these configurations following a sudden temperature jump into the liquid phase. In homogeneous geometries, we find that enhanced kinetic stability is accompanied by large scale dynamic heterogeneity, while a competition between homogeneous and heterogeneous melting is observed when a liquid boundary invades the glass at constant velocity. Our work demonstrates the feasibility of large-scale, atomistically resolved, and experimentally relevant simulations of the kinetics of ultrastable glasses.

Authors:

Hocky, Glen M.; Reichman, David R. ^[1]; Berthier, Ludovic ^[2]

Department of Chemistry, Columbia University, 3000 Broadway, New York, New York 10027 (United States)
Laboratoire Charles Coulomb, UMR 5221, CNRS and Université Montpellier 2, Montpellier (France)

Publication Date:: Sun Dec 14 00:00:00 EST 2014

OSTI Identifier:: 22413304

Resource Type:: Journal Article

Journal Name:: Journal of Chemical Physics

Additional Journal Information:: Journal Volume: 141; Journal Issue: 22; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; GLASS; KINETICS; LIQUIDS; MELTING; NUMERICAL ANALYSIS; SIMULATION; STABILITY; VAPOR DEPOSITED COATINGS

Citation Formats


                    Hocky, Glen M., Reichman, David R., and Berthier, Ludovic. Equilibrium ultrastable glasses produced by random pinning.  United States: N. p., 2014. 
        Web.  doi:10.1063/1.4903200.

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                    Hocky, Glen M., Reichman, David R., & Berthier, Ludovic. Equilibrium ultrastable glasses produced by random pinning.  United States.  https://doi.org/10.1063/1.4903200

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                    Hocky, Glen M., Reichman, David R., and Berthier, Ludovic. 2014.  
        "Equilibrium ultrastable glasses produced by random pinning".  United States.  https://doi.org/10.1063/1.4903200.

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@article{osti_22413304,

  title        = {Equilibrium ultrastable glasses produced by random pinning},

  author       = {Hocky, Glen M. and Reichman, David R. and Berthier, Ludovic},

  abstractNote = {Ultrastable glasses have risen to prominence due to their potentially useful material properties and the tantalizing possibility of a general method of preparation via vapor deposition. Despite the importance of this novel class of amorphous materials, numerical studies have been scarce because achieving ultrastability in atomistic simulations is an enormous challenge. Here, we bypass this difficulty and establish that randomly pinning the position of a small fraction of particles inside an equilibrated supercooled liquid generates ultrastable configurations at essentially no numerical cost, while avoiding undesired structural changes due to the preparation protocol. Building on the analogy with vapor-deposited ultrastable glasses, we study the melting kinetics of these configurations following a sudden temperature jump into the liquid phase. In homogeneous geometries, we find that enhanced kinetic stability is accompanied by large scale dynamic heterogeneity, while a competition between homogeneous and heterogeneous melting is observed when a liquid boundary invades the glass at constant velocity. Our work demonstrates the feasibility of large-scale, atomistically resolved, and experimentally relevant simulations of the kinetics of ultrastable glasses.},

  doi          = {10.1063/1.4903200},

  url          = {https://www.osti.gov/biblio/22413304},
  journal      = {Journal of Chemical Physics},

  issn         = {0021-9606},

  number       = 22,

  volume       = 141,

  place        = {United States},

  year         = {Sun Dec 14 00:00:00 EST 2014},

  month        = {Sun Dec 14 00:00:00 EST 2014}

}

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