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Kinetic crystallisation instability in liquids with short-ranged attractions

Research output: Contribution to journalSpecial issue

Original languageEnglish
Pages (from-to)3076-3084
Number of pages7
JournalMolecular Physics
Volume116
Issue number21-22
Early online date3 Jul 2018
DOIs
DateAccepted/In press - 7 Jun 2018
DateE-pub ahead of print - 3 Jul 2018
DatePublished (current) - 17 Nov 2018

Abstract

Liquids in systems with spherically symmetric interactions are not thermodynamically stable when the range of the attraction is reduced sufficiently. However, these metastable liquids have lifetimes long enough that they are readily observable prior to crystallisation. Here we investigate the fate of liquids when the interaction range is reduced dramatically. Under these conditions, we propose that the liquid becomes kinetically unstable, i.e. its properties are non-stationary on the timescale of structural relaxation. Using molecular dynamics simulations, we find that in the square well model with range 6% of the diameter, the liquid crystallises within the timescale of structural relaxation for state points except those so close to criticality that the lengthscale of density fluctuations couples to the length of the simulation box size for typical system sizes. Even very close to criticality, the liquid exhibits significant structural change on the timescale of relaxation.

    Research areas

  • Crystallisation, liquid structure, simple liquids

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  • Full-text PDF (accepted author manuscript)

    Rights statement: This is the author accepted manuscript (AAM). The final published version (version of record) is available online via Taylor & Francis at https://www.tandfonline.com/doi/full/10.1080/00268976.2018.1492743 . Please refer to any applicable terms of use of the publisher.

    Accepted author manuscript, 2.49 MB, PDF document

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