Structural relaxation dynamics in binary glass-forming molecular liquids with ideal and complex mixing behavior.

The glass transition and structural relaxation dynamics of various binary glass-forming liquids are investigated with dielectric relaxation measurements across the entire composition range. Three categories of solutions with weak, intermediate, and strong mixing effects, namely methyl-m-toluate in methyl o-toluate, methyl m-toluate in di-n-butyl phthalate, and 1,2-propandiol in 2-hexylamine, are selected to address the mixing behaviors from near-ideal to nonideal cases. The glass transition temperatures, fragility indices, and stretching exponents of the solutions are determined and their composition dependence is the focus of this study. The experimental measurements show that mixing generally generates a negative deviation of fragility m relative to the composition average of the results of two neat components (ideal mixing law). This excess negative fragility proves to be a universal feature of binary systems, and the increase of the nonideal mixing degree results in a more pronounced negative deviation. In contrast, the composition dependence of the stretching exponents is more complex, and a transition from the negative to positive deviation is observed for substantial nonideal character. The study assists understanding the dynamics of multicomponent glass formers.