Two factors governing fragility: Stretching exponent and configurational entropy
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Abstract
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 β 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 β 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 β and fragility and those who question such a correlation due to the spread of the data.