Experimental evidence of a crossover between cooperative relaxation and liquid growth dynamics

Abstract: In stark contrast with the conventional understanding of the glass transition, where the transition from glass to liquid appears as a dynamic process where atoms/molecules cooperatively relax into the equilibrium phase, we experimentally show that the nature of the glass transition depends at a given temperature on the ratio between the relaxation time of the glass, {\tau}glass, taken as its transformation time, and the alpha relaxation time, {\tau}{\alpha}. Although the relaxation of liquid-cooled glasses is not totally synchronous, due to the existence of a distribution of relaxation times, there has been no clear observation of phase separation. However, at temperatures at which {\tau}glass/{\tau}{\alpha} is large, high mobility regions nucleate into the liquid phase that subsequently grow by dynamic facilitation before, or while, cooperative glass relaxation sets into play. On the contrary, at temperatures associated to smaller {\tau}glass/{\tau}{\alpha} the glass transition proceeds by cooperative relaxation dynamics all across the material. This behavior is independent of the experimental procedure or protocol to produce the glass.