4.8 Article

Avalanches mediate crystallization in a hard-sphere glass

Publisher

NATL ACAD SCIENCES
DOI: 10.1073/pnas.1308338110

Keywords

colloidal glasses; ordered solid; amorphous solid; dynamic heterogeneities

Funding

  1. Intra-European Marie Curie Fellowship [237443-HINECOP-FP7-PEOPLE-IEF-2008, 237454-ACSELFASSEMBLY-FP7-PEOPLE-IEF-2008]
  2. Marie Curie Career Integration Grant [322326-COSAACFP7-PEOPLE-CIG-2012, 303941-ANISOKINEQ-FP7-PEOPLE-CIG-2011]
  3. Juan de La Cierva Spanish Fellowship [JCI-2010-06602]
  4. Ramon y Cajal Spanish Fellowship [RYC-2010-06098]
  5. Spanish National Project [FIS2010-16159]
  6. FIRB program of the Ministero dell' Istruzione, dell'Universita' e della Ricerca [RBFR125H0M]
  7. Engineering and Physical Sciences Research Council [EP/J007404]
  8. Royal Society Research Professorship
  9. eScience Data Information and Knowledge Transformation initiative
  10. [ITN-234810-COMPLOIDS]
  11. EPSRC [EP/J007404/1] Funding Source: UKRI
  12. Engineering and Physical Sciences Research Council [EP/J007404/1] Funding Source: researchfish

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By molecular-dynamics simulations, we have studied the devitrification (or crystallization) of aged hard-sphere glasses. First, we find that the dynamics of the particles are intermittent: Quiescent periods, when the particles simply rattle in their nearest-neighbor cages, are interrupted by abrupt avalanches, where a subset of particles undergo large rearrangements. Second, we find that crystallization is associated with these avalanches but that the connection is not straightforward. The amount of crystal in the system increases during an avalanche, but most of the particles that become crystalline are different from those involved in the avalanche. Third, the occurrence of the avalanches is a largely stochastic process. Randomizing the velocities of the particles at any time during the simulation leads to a different subsequent series of avalanches. The spatial distribution of avalanching particles appears random, although correlations are found among avalanche initiation events. By contrast, we find that crystallization tends to take place in regions that already show incipient local order.

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