Crystallization Instability in Glass-Forming Mixtures

Research output: Contribution to journalJournal articleResearchpeer-review

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).
Original languageEnglish
Article number031016
JournalPhysical Review X
Volume9
Issue number3
Number of pages11
ISSN2160-3308
DOIs
Publication statusPublished - 2019

Cite this

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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}",
year = "2019",
doi = "10.1103/PhysRevX.9.031016",
language = "English",
volume = "9",
journal = "Physical Review X",
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publisher = "American Physical Society",
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}

Crystallization Instability in Glass-Forming Mixtures. / Ingebrigtsen, Trond; Dyre, Jeppe; Schrøder, Thomas; Royall, C. Patrick .

In: Physical Review X, Vol. 9, No. 3, 031016, 2019.

Research output: Contribution to journalJournal articleResearchpeer-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).

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DO - 10.1103/PhysRevX.9.031016

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JO - Physical Review X

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