Computing the viscosity of supercooled liquids. II. Silica and strong-fragile crossover behavior

Akihiro Kushima, Xi Lin, Ju Li, Xiaofeng Qian, Jacob Eapen, John C. Mauro, Phong Diep, Sidney Yip

Research output: Contribution to journalArticle

34 Citations (Scopus)

Abstract

A recently developed atomistic method capable of calculating the fragile (non-Arrhenius) temperature behavior of highly viscous liquids is further tested by studying a model of SiO2, a glass former well known for its Arrhenius temperature behavior (strong). The method predicts an Arrhenius temperature variation, in agreement with experiments, the origin of which is revealed by both quantitative and qualitative results on transition state pathways, activation barrier analysis, energy landscape connectivity, and atomistic activation mechanisms. Also predicted is a transition from fragile to strong behavior at a lower viscosity, below the range of measurements, which had been previously suggested on the basis of molecular dynamics simulations. By systematically comparing our findings with corresponding results on the binary Lennard-Jones system (fragile) we gain new insights into the topographical features of the potential energy landscape, characteristics that distinguish strong from fragile glassy systems. We interpret fragility as a universal manifestation of slowing of dynamics when the system becomes trapped in deep energy basins. As a consequence, all glass-forming systems, when cooled from their normal liquid state, should exhibit two transitions in temperature scaling of the viscosity, a strong-to-fragile crossover followed by a second transition reverting back to strong behavior.

Original languageEnglish (US)
Article number164505
JournalJournal of Chemical Physics
Volume131
Issue number16
DOIs
StatePublished - Dec 21 2009

Fingerprint

Viscosity of liquids
Silicon Dioxide
crossovers
viscosity
silicon dioxide
liquids
Chemical activation
activation
Viscosity
Glass
Temperature
temperature
glass
Liquids
Potential energy
Molecular dynamics
potential energy
molecular dynamics
scaling
energy

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Kushima, Akihiro ; Lin, Xi ; Li, Ju ; Qian, Xiaofeng ; Eapen, Jacob ; Mauro, John C. ; Diep, Phong ; Yip, Sidney. / Computing the viscosity of supercooled liquids. II. Silica and strong-fragile crossover behavior. In: Journal of Chemical Physics. 2009 ; Vol. 131, No. 16.
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Computing the viscosity of supercooled liquids. II. Silica and strong-fragile crossover behavior. / Kushima, Akihiro; Lin, Xi; Li, Ju; Qian, Xiaofeng; Eapen, Jacob; Mauro, John C.; Diep, Phong; Yip, Sidney.

In: Journal of Chemical Physics, Vol. 131, No. 16, 164505, 21.12.2009.

Research output: Contribution to journalArticle

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