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Supercooled liquids and the glass transition

Nature volume 410, pages 259–267 (2001)Cite this article

Abstract

Glasses are disordered materials that lack the periodicity of crystals but behave mechanically like solids. The most common way of making a glass is by cooling a viscous liquid fast enough to avoid crystallization. Although this route to the vitreous state — supercooling — has been known for millennia, the molecular processes by which liquids acquire amorphous rigidity upon cooling are not fully understood. Here we discuss current theoretical knowledge of the manner in which intermolecular forces give rise to complex behaviour in supercooled liquids and glasses. An intriguing aspect of this behaviour is the apparent connection between dynamics and thermodynamics. The multidimensional potential energy surface as a function of particle coordinates (the energy landscape) offers a convenient viewpoint for the analysis and interpretation of supercooling and glass-formation phenomena. That much of this analysis is at present largely qualitative reflects the fact that precise computations of how viscous liquids sample their landscape have become possible only recently.

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Figure 1: Temperature dependence of a liquid's volume v or enthalpy h at constant pressure.
Figure 2: Tg-scaled Arrhenius representation of liquid viscosities showing Angell's strong–fragile pattern.
Figure 3: Temperature dependence of the peak dielectric relaxation frequency of the glass-forming mixture chlorobenzene/cis-decalin (molar ratio 17.2/82.8%).
Figure 4: Temperature dependence of the entropy difference between several supercooled liquids and their stable crystals at atmospheric pressure.
Figure 5: Schematic illustration of an energy landscape.
Figure 6: Mean inherent structure energy per particle of a binary mixture of unequal-sized Lennard–Jones atoms, as a function of the temperature of the equilibrated liquid from which the inherent structures were generated by energy minimization.
Figure 7: Relationship between diffusivity (D) and configurational entropy (Sconf) of supercooled water79 at six different temperatures.
Figure 8: Schematic representation of the energy landscapes of strong and fragile substances.
Figure 9: Evolution of the self-intermediate scattering function for A-type atoms for the same supercooled Lennard–Jones mixture as in Fig. 6, at q σAA = 7.251, corresponding to the first peak of the static structure factor of species A (ref. 92).

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Acknowledgements

P.G.D.'s work is supported by the US Department of Energy.

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  1. Department of Chemical Engineering, Princeton University, Princeton, 08544, New Jersey, USA

    Pablo G. Debenedetti

  2. Princeton Materials Institute, Princeton University, Princeton, 08544, New Jersey, USA

    Frank H. Stillinger

  3. Bell Laboratories, Lucent Technologies, Murray Hill, 07974, New Jersey, USA

    Frank H. Stillinger

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Debenedetti, P., Stillinger, F. Supercooled liquids and the glass transition. Nature 410, 259–267 (2001). https://doi.org/10.1038/35065704

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