Crystallization Instability in Glass-Forming Mixtures

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningpeer review

Resumé

Understanding the mechanisms by which crystal nuclei form is crucial for many phenomena such as
gaining control over crystallization in glass-forming materials or accurately modeling rheological behavior of
magma flows. The microscopic nature of such nuclei, however, makes their understanding extremely hard in
experiments, while computer simulations have hitherto been hampered by short timescales and small system
sizes. Here we use highly efficient graphics processing unit simulation techniques to address these challenges.
The larger systems we access reveal a general nucleation mechanism in mixtures. In particular, we find that
the supercooled liquid of a prized atomistic model glass former (Kob-Andersen model) is inherently unstable
to crystallization, i.e., that nucleation is unavoidable on the structural relaxation timescale, for system sizes of
10 000 particles and larger. This is due to compositional fluctuations leading to regions composed of one
species that are larger than the critical nucleus of that species, which rapidly crystallize. We argue that this
mechanism provides a minimum rate of nucleation in mixtures in general, and show that the same mechanism
pertains to the metallic glass former copper zirconium (CuZr).
OriginalsprogEngelsk
Artikelnummer031016
TidsskriftPhysical Review X
Vol/bind9
Udgave nummer3
Antal sider11
ISSN2160-3308
DOI
StatusUdgivet - 2019

Citer dette

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title = "Crystallization Instability in Glass-Forming Mixtures",
abstract = "Understanding the mechanisms by which crystal nuclei form is crucial for many phenomena such as gaining control over crystallization in glass-forming materials or accurately modeling rheological behavior of magma flows. The microscopic nature of such nuclei, however, makes their understanding extremely hard in experiments, while computer simulations have hitherto been hampered by short timescales and small system sizes. Here we use highly efficient graphics processing unit simulation techniques to address these challenges. The larger systems we access reveal a general nucleation mechanism in mixtures. In particular, we find that the supercooled liquid of a prized atomistic model glass former (Kob-Andersen model) is inherently unstable to crystallization, i.e., that nucleation is unavoidable on the structural relaxation timescale, for system sizes of 10 000 particles and larger. This is due to compositional fluctuations leading to regions composed of one species that are larger than the critical nucleus of that species, which rapidly crystallize. We argue that this mechanism provides a minimum rate of nucleation in mixtures in general, and show that the same mechanism pertains to the metallic glass former copper zirconium (CuZr).",
author = "Trond Ingebrigtsen and Jeppe Dyre and Thomas Schr{\o}der and Royall, {C. Patrick}",
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doi = "10.1103/PhysRevX.9.031016",
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Crystallization Instability in Glass-Forming Mixtures. / Ingebrigtsen, Trond; Dyre, Jeppe; Schrøder, Thomas; Royall, C. Patrick .

I: Physical Review X, Bind 9, Nr. 3, 031016, 2019.

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningpeer review

TY - JOUR

T1 - Crystallization Instability in Glass-Forming Mixtures

AU - Ingebrigtsen, Trond

AU - Dyre, Jeppe

AU - Schrøder, Thomas

AU - Royall, C. Patrick

PY - 2019

Y1 - 2019

N2 - Understanding the mechanisms by which crystal nuclei form is crucial for many phenomena such as gaining control over crystallization in glass-forming materials or accurately modeling rheological behavior of magma flows. The microscopic nature of such nuclei, however, makes their understanding extremely hard in experiments, while computer simulations have hitherto been hampered by short timescales and small system sizes. Here we use highly efficient graphics processing unit simulation techniques to address these challenges. The larger systems we access reveal a general nucleation mechanism in mixtures. In particular, we find that the supercooled liquid of a prized atomistic model glass former (Kob-Andersen model) is inherently unstable to crystallization, i.e., that nucleation is unavoidable on the structural relaxation timescale, for system sizes of 10 000 particles and larger. This is due to compositional fluctuations leading to regions composed of one species that are larger than the critical nucleus of that species, which rapidly crystallize. We argue that this mechanism provides a minimum rate of nucleation in mixtures in general, and show that the same mechanism pertains to the metallic glass former copper zirconium (CuZr).

AB - Understanding the mechanisms by which crystal nuclei form is crucial for many phenomena such as gaining control over crystallization in glass-forming materials or accurately modeling rheological behavior of magma flows. The microscopic nature of such nuclei, however, makes their understanding extremely hard in experiments, while computer simulations have hitherto been hampered by short timescales and small system sizes. Here we use highly efficient graphics processing unit simulation techniques to address these challenges. The larger systems we access reveal a general nucleation mechanism in mixtures. In particular, we find that the supercooled liquid of a prized atomistic model glass former (Kob-Andersen model) is inherently unstable to crystallization, i.e., that nucleation is unavoidable on the structural relaxation timescale, for system sizes of 10 000 particles and larger. This is due to compositional fluctuations leading to regions composed of one species that are larger than the critical nucleus of that species, which rapidly crystallize. We argue that this mechanism provides a minimum rate of nucleation in mixtures in general, and show that the same mechanism pertains to the metallic glass former copper zirconium (CuZr).

U2 - 10.1103/PhysRevX.9.031016

DO - 10.1103/PhysRevX.9.031016

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JO - Physical Review X

JF - Physical Review X

SN - 2160-3308

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ER -