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

Nature volume 412, pages 514–517 (2001)Cite this article

Abstract

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 temperature1,2. In contrast, most liquids are to some degree ‘fragile’, showing significantly faster increases in their viscosity as the glass transition temperature is approached. Recent studies3,4,5,6,35,36 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.

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Figure 1: Variation of inherent structure energy eIS with temperature T.
Figure 2: Entropy S and its component contributions as a function of temperature.
Figure 3: Relationship of diffusion coefficient D to temperature T and configurational entropy Sc.
Figure 4: Potential energy U and isochoric specific heat CV as a function of T.

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Acknowledgements

We thank C. A. Angell, W. Kob, S. Sastry and R. Speedy for discussions. I.S.-V. and P.H.P. thank NSERC (Canada) for financial support, and SHARCNET for computing resources. F.S. acknowledges support from the INFM ‘Iniziativa Calcolo Parallelo’ and PRE-HOP and from MURST PRIN 2000.

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Authors and Affiliations

  1. Department of Applied Mathematics, University of Western Ontario, London, N6A 5B7, Ontario, Canada

    Ivan Saika-Voivod & Peter H. Poole

  2. Dipartimento di Fisica and Istituto Nazionale per la Fisica della Materia, Universita' di Roma La Sapienza, Piazzale Aldo Moro 2, Rome, I-00185, Italy

    Francesco Sciortino

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  1. Ivan Saika-Voivod
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Correspondence to Peter H. Poole.

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Saika-Voivod, I., Poole, P. & Sciortino, F. Fragile-to-strong transition and polyamorphism in the energy landscape of liquid silica. Nature 412, 514–517 (2001). https://doi.org/10.1038/35087524

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