Two factors governing fragility: stretching exponent and configurational entropy.
We derive an analytical expression showing that the fragility of a supercooled liquid is a result of (i) a thermodynamic term depending on change in configurational entropy and (ii) a kinetic term depending on change in the nonexponentiality or "stretching" of the relaxation function, as quantified by the exponent beta of the Kohlrausch-Williams-Watts (KWW) relaxation function. Our expression indicates that there is not a direct correlation between the non-Arrhenius scaling of liquid viscosity and the nonexponential nature of glassy relaxation. Rather, the temperature dependence of the stretching exponent beta provides a lower limit for fragility, which can be increased through changes in the configurational entropy. Our result explains the apparent contradiction between those researchers showing a correlation between beta and fragility and those who question such a correlation due to the spread of the data.
Gupta
Prabhat K
PK
Department of Materials Science and Engineering, The Ohio State University, Columbus, Ohio 43210, USA.
Mauro
John C
JC