Fragile-to-strong transition and polyamorphism in the energy landscape of liquid silica

Article

关键词: CONFIGURATIONAL ENTROPY;    SUPERCOOLED LIQUIDS;    GLASS-TRANSITION;    VISCOUS SILICA;    RELAXATION;    VISCOSITY;    WATER;    MODEL;   

DOI  :  10.1038/35087524

来源: SCIE

【 摘 要 】

Liquid silica is the archetypal glass former, and compounds based on silica are ubiquitous as natural and man-made amorphous materials. Liquid silica is also the extreme case of a 'strong' liquid, in that the variation of viscosity with temperature closely follows the Arrhenius law as the liquid is cooled toward its glass transition temperature(1,2). In contrast, most liquids are to some degree 'fragile', showing significantly faster increases in their viscosity as the glass transition temperature is approached. Recent studies(3-6,35,36) have demonstrated the controlling influence of the potential energy hypersurface (or 'energy landscape') of the liquid on the transport properties near the glass transition. But the origin of strong liquid behaviour in terms of the energy landscape has not yet been resolved. Here we study the static and dynamic properties of liquid silica over a wide range of temperature and density using computer simulations. The results reveal a change in the energy landscape with decreasing temperature, which underlies a transition from a fragile liquid at high temperature to a strong liquid at low temperature. We also show that a specific heat anomaly is associated with this fragile-to-strong transition, and suggest that this anomaly is related to the polyamorphic behaviour of amorphous solid silica.

【 授权许可】

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