An upper limit to kinetic fragility in glass-forming liquids

Abstract

The kinetic fragility of a liquid is correlated to the magnitude of enthalpy hysteresis in various glass-forming materials during thermal cycling across the glass transition. While the lower bound of liquid fragility is well known, there has been little research into the possibility of an inherent upper limit to fragility. In this paper, we present a theoretical argument for the existence of a maximum fragility and show that the correlation between fragility and enthalpy hysteresis allows for an empirical evaluation of the upper limit of fragility. This upper limit occurs as the enthalpy hysteresis involved in thermal cycling about the glass transition approaches zero, leading to m(max)≈175. This result agrees remarkably well with our previous estimate. The dynamics of maximum fragility liquids are discussed, and a critical temperature of ∼1.5 T(g) (where T(g) is the glass transition temperature) is revealed where a transition from nonexponential to exponential structural relaxation occurs.