Equilibrium ultrastable glasses produced by random pinning

Glen Hocky, Ludovic Berthier, David R. Reichman

Research output: Contribution to journalArticle

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.

Original languageEnglish (US)
Article number224503
JournalJournal of Chemical Physics
Volume141
Issue number22
DOIs
StatePublished - Jan 1 2014

Fingerprint

Glass
glass
Kinetics
kinetics
Liquids
Melting
melting
preparation
Vapor deposition
bypasses
amorphous materials
liquids
configurations
Materials properties
liquid phases
simulation
Vapors
vapor deposition
vapors
costs

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Equilibrium ultrastable glasses produced by random pinning. / Hocky, Glen; Berthier, Ludovic; Reichman, David R.

In: Journal of Chemical Physics, Vol. 141, No. 22, 224503, 01.01.2014.

Research output: Contribution to journalArticle

Hocky, Glen ; Berthier, Ludovic ; Reichman, David R. / Equilibrium ultrastable glasses produced by random pinning. In: Journal of Chemical Physics. 2014 ; Vol. 141, No. 22.
@article{1a63df6b950b42c7b2fea01fb79a4f66,
title = "Equilibrium ultrastable glasses produced by random pinning",
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.",
author = "Glen Hocky and Ludovic Berthier and Reichman, {David R.}",
year = "2014",
month = "1",
day = "1",
doi = "10.1063/1.4903200",
language = "English (US)",
volume = "141",
journal = "Journal of Chemical Physics",
issn = "0021-9606",
publisher = "American Institute of Physics Publising LLC",
number = "22",

}

TY - JOUR

T1 - Equilibrium ultrastable glasses produced by random pinning

AU - Hocky, Glen

AU - Berthier, Ludovic

AU - Reichman, David R.

PY - 2014/1/1

Y1 - 2014/1/1

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=84916216666&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84916216666&partnerID=8YFLogxK

U2 - 10.1063/1.4903200

DO - 10.1063/1.4903200

M3 - Article

AN - SCOPUS:84916216666

VL - 141

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

SN - 0021-9606

IS - 22

M1 - 224503

ER -