A Topographic View of Supercooled Liquids and Glass Formation

@article{Stillinger1995ATV,
  title={A Topographic View of Supercooled Liquids and Glass Formation},
  author={Frank H. Stillinger},
  journal={Science},
  year={1995},
  volume={267},
  pages={1935 - 1939}
}
Various static and dynamic phenomena displayed by glass-forming liquids, particularly those near the so-called "fragile" limit, emerge as manifestations of the multidimensional complex topography of the collective potential energy function. These include non-Arrhenius viscosity and relaxation times, bifurcation between the α- and β-relaxation processes, and a breakdown of the Stokes-Einstein relation for self-diffusion. This multidimensional viewpoint also produces an extension of the venerable… Expand
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References

SHOWING 1-10 OF 24 REFERENCES
Relaxation behavior in atomic and molecular glasses.
  • Stillinger
  • Physics, Medicine
  • Physical review. B, Condensed matter
  • 1990
TLDR
The objective of this paper is to relate a and ~ to gross topographical features of the many-particle potential-energy hypersurface and to conclude that a should decline with decreasing temperature. Expand
Supercooled liquids, glass transitions, and the Kauzmann paradox
Many liquids have heat capacities that substantially exceed those of the corresponding crystal, and this discrepancy magnifies in the supercooled regime. Thus, liquid entropy declines more rapidlyExpand
Nonexponential relaxations in strong and fragile glass formers
Deviations from thermally activated and from exponential response are typical features of the vitrification phenomenon and previously have been studied using viscoelastic, dielectric, calorimetric,Expand
Models of the glass transition
The different physical aspects of glass transitions are reviewed and models aiming at their explanation are described. The following three main aspects are distinguished: the degree of stability ofExpand
Viscous Liquids and the Glass Transition: A Potential Energy Barrier Picture
Recent attempts have been made to assess the relative merits of the free volume and entropy theories of viscous flow in glass‐forming liquids by accurate measurement of viscosity over wideExpand
Multidimensional geometric aspects of the solid–liquid transition in simple substances
Any molecular system explores significantly different regions of the potential‐energy hypersurface as the system is found, respectively, in the solid and liquid phases. We study in detail theExpand
Viscous liquids and the glass transition. VII. Molecular mechanisms for a thermodynamic second order transition
It has been previously shown that the ’’configurational’’ specific heat ΔCp of a liquid above Tg contains significant contributions from nonconfigurational sources such as changes with structuralExpand
Translation-rotation paradox for diffusion in fragile glass-forming liquids.
  • Stillinger, Hodgdon
  • Physics, Medicine
  • Physical review. E, Statistical physics, plasmas, fluids, and related interdisciplinary topics
  • 1994
TLDR
Owing to a suitable combination of domain parameters (mean size, lifetime, concentration, internal viscosity), the observed diffusion rate discrepancy can indeed be rationalized. Expand
Hidden structure in liquids
The canonical partition function for classical many-body systems is transformed so that the temperature-independent packing statistics and the thermal excitations are uniquely separated. ThisExpand
The Microscopic Basis of the Glass Transition in Polymers from Neutron Scattering Studies
TLDR
The connection between this boson peak and the fast dynamic process appearing near Tg is discussed, and the time-temperature superposition principle, which is valid for polymers on a macroscopic scale, is not applicable for temperatures approaching Tg. Expand
...
1
2
3
...