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Direct observation of a local structural mechanism for dynamic arrest

Royall, C. Patrick; Williams, Stephen; Ohtsuka, Takehiro; Tanaka, Hajime

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The mechanism by which a liquid may become arrested, forming a glass or gel, is a long-standing problem of materials science. In particular, long-lived (energetically) locally favoured structures (LFSs), the geometry of which may prevent the system relaxing to its equilibrium state, have long been thought to play a key role in dynamical arrest. Here, we propose a definition of LFSs which we identify with a novel topological method and directly measure with experiments on a colloidal liquid-gel...[Show more]

dc.contributor.authorRoyall, C. Patrick
dc.contributor.authorWilliams, Stephen
dc.contributor.authorOhtsuka, Takehiro
dc.contributor.authorTanaka, Hajime
dc.date.accessioned2015-12-10T22:25:07Z
dc.identifier.issn1476-1122
dc.identifier.urihttp://hdl.handle.net/1885/53342
dc.description.abstractThe mechanism by which a liquid may become arrested, forming a glass or gel, is a long-standing problem of materials science. In particular, long-lived (energetically) locally favoured structures (LFSs), the geometry of which may prevent the system relaxing to its equilibrium state, have long been thought to play a key role in dynamical arrest. Here, we propose a definition of LFSs which we identify with a novel topological method and directly measure with experiments on a colloidal liquid-gel transition. The population of LFSs is a strong function of (effective) temperature in the ergodic liquid phase, rising sharply approaching dynamical arrest, and indeed forms a percolating network that becomes the arms of the gel. Owing to the LFSs, the gel is unable to reach equilibrium, crystal-gas coexistence. Our results provide direct experimental observation of a link between local structure and dynamical arrest, and open a new perspective on a wide range of metastable materials.
dc.publisherNature Publishing Group
dc.sourceNature Materials
dc.subjectKeywords: Colloids; Computer networks; Dynamical systems; Fluids; Gelation; Gels; Growth (materials); Interfaces (materials); Liquid phase epitaxy; Materials; Mechanics; Mechanisms; Metropolitan area networks; Network protocols; Pigments; Structure (composition); (
dc.titleDirect observation of a local structural mechanism for dynamic arrest
dc.typeJournal article
local.description.notesImported from ARIES
local.identifier.citationvolume7
dc.date.issued2008
local.identifier.absfor030704 - Statistical Mechanics in Chemistry
local.identifier.ariespublicationu4217927xPUB271
local.type.statusPublished Version
local.contributor.affiliationRoyall, C. Patrick, University of Bristol
local.contributor.affiliationWilliams, Stephen, College of Physical and Mathematical Sciences, ANU
local.contributor.affiliationOhtsuka, Takehiro, University of Tokyo
local.contributor.affiliationTanaka, Hajime, University of Tokyo
local.description.embargo2037-12-31
local.bibliographicCitation.issue7
local.bibliographicCitation.startpage556
local.bibliographicCitation.lastpage561
local.identifier.doi10.1038/nmat2219
dc.date.updated2015-12-09T09:21:25Z
local.identifier.scopusID2-s2.0-45849092542
local.identifier.thomsonID000257072800019
CollectionsANU Research Publications

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