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Common mechanism of thermodynamic and mechanical origin for ageing and crystallization of glasses

Abstract:
The glassy state is known to undergo slow structural relaxation, where the system progressively explores lower free-energy minima which are either amorphous (ageing) or crystalline (devitrification). Recently, there is growing interest in the unusual intermittent collective displacements of a large number of particles known as ‘avalanches’. However, their structural origin and dynamics are yet to be fully addressed. Here, we study hard-sphere glasses which either crystallize or age depending on the degree of size polydispersity, and show that a small number of particles are thermodynamically driven to rearrange in regions of low density and bond orientational order. This causes a transient loss of mechanical equilibrium which facilitates a large cascade of motion. Combined with previously identified phenomenology, we have a complete kinetic pathway for structural change which is common to both ageing and crystallization. Furthermore, this suggests that transient force balance is what distinguishes glasses from supercooled liquids.
Publication status:
Published
Peer review status:
Peer reviewed

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Publisher copy:
10.1038/ncomms15954

Authors


More by this author
Institution:
University of Oxford
Division:
MPLS
Department:
Chemistry
Sub department:
Physical & Theoretical Chem
Role:
Author
ORCID:
0000-0002-7511-1958
More by this author
Role:
Author
ORCID:
0000-0002-4444-1890


Publisher:
Nature Research
Journal:
Nature Communications More from this journal
Volume:
8
Article number:
15954
Publication date:
2017-08-29
Acceptance date:
2017-05-17
DOI:
EISSN:
2041-1723
Pmid:
28660879


Language:
English
Keywords:
Pubs id:
pubs:844509
UUID:
uuid:21552a7c-02d2-4cb3-9c17-4154369713db
Local pid:
pubs:844509
Source identifiers:
844509
Deposit date:
2019-05-17

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