TY - JOUR
T1 - Perspective on the glass transition
AU - Angell, C. A.
N1 - Funding Information:
Acknowledgements-The writer acknowledgess upport of this work by the National ScienceF oundationu nderS olid State Chemistry Grant No. DMR 8304887a, nd helpful discussionsw ith J. Jackie, L. M. Torell, and S. Yip.
PY - 1988
Y1 - 1988
N2 - Some of the reasons for the current interest in the phenomenology of vitrification are reviewed and progress due to, as well as limitations of, mode coupling theories (MCT) for viscosity divergence are examined. Liquids which fit the MCT predictions best are also those with the most imminent Kauzmann entropy crises near the glass transition temperature, Tg. Mode coupling predictions break down far above Tg at the point, Tx, where Goldstein long ago argued that activated processes controlled by the (3N + 1)-dimensional potential energy surface for the N- particle system should become dominant. Examining behavior in the energy topology-controlled regime, we note that ergodicity-breaking is not simply a consequence of viscosity divergence. In the liquids best fitting MCT, which are at the fragile extreme of liquid behavior, shear and structural relaxation processes slowly decouple below Tx, leading to breakdown of the Adam-Gibbs equation for viscosity. The latter in its original and derived Vogel-Fulcher forms remains valid for enthalpy (and presumably volume) relaxation processes. The distinction between strong and fragile behavior in liquids is related to the density of configurational states (minima) characterizing the potential energy surface.
AB - Some of the reasons for the current interest in the phenomenology of vitrification are reviewed and progress due to, as well as limitations of, mode coupling theories (MCT) for viscosity divergence are examined. Liquids which fit the MCT predictions best are also those with the most imminent Kauzmann entropy crises near the glass transition temperature, Tg. Mode coupling predictions break down far above Tg at the point, Tx, where Goldstein long ago argued that activated processes controlled by the (3N + 1)-dimensional potential energy surface for the N- particle system should become dominant. Examining behavior in the energy topology-controlled regime, we note that ergodicity-breaking is not simply a consequence of viscosity divergence. In the liquids best fitting MCT, which are at the fragile extreme of liquid behavior, shear and structural relaxation processes slowly decouple below Tx, leading to breakdown of the Adam-Gibbs equation for viscosity. The latter in its original and derived Vogel-Fulcher forms remains valid for enthalpy (and presumably volume) relaxation processes. The distinction between strong and fragile behavior in liquids is related to the density of configurational states (minima) characterizing the potential energy surface.
KW - Glass transition
KW - Kauzmann paradox
KW - configurational states
KW - mode coupling
KW - viscosity divergence
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U2 - 10.1016/0022-3697(88)90002-9
DO - 10.1016/0022-3697(88)90002-9
M3 - Article
AN - SCOPUS:0023871743
SN - 0022-3697
VL - 49
SP - 863
EP - 871
JO - Journal of Physics and Chemistry of Solids
JF - Journal of Physics and Chemistry of Solids
IS - 8
ER -