Crossing the Frontier of Validity of the Material Time Approach in the Aging of a Molecular Glass.

Abstract

We studied the physical aging of glycerol in response to upward temperature steps of amplitude ranging from 0.3 to 18 K. This was done using a specially designed experimental setup allowing quick heating of a liquid film while measuring the evolution of its dielectric properties. Despite the nonlinear evolution of these observables for large steps, a fictive temperature could be obtained. In the case of moderate step amplitudes, we checked that the material time approach in its simplest form, the single parameter aging (SPA), applies well. The memory kernel extracted from the quasi-linear regime was used to test its frontiers of validity for significant step amplitudes. We showed that the observations deviate from the prediction of the material time framework and of SPA simultaneously. As these approaches link aging to equilibrium dynamics, our results help set the bounds beyond which new theoretical arguments are needed.