Dynamics of glass-forming liquids. XVI. Observation of ultrastable glass transformation via dielectric spectroscopy

The transformation of vapor-deposited ultrastable glasses of indomethacin (IMC) into the supercooled liquid state near T_g is monitored by means of dielectric spectroscopy. Films with thickness between 400 and 800 nm are deposited on differential interdigitated electrode cells and their loss profiles are measured during isothermal annealing using a dual-channel impedance technique for frequencies between 0.03 and 100 Hz. All dielectric loss spectra observed during the transformation process can be explained by a volume fraction of the supercooled liquid that increases linearly with time. From the early stages of the transformation to the liquid that is formed via complete annealing of the ultrastable glass, the average dielectric relaxation time as well as the distribution of relaxation times of the liquid component are identical to those of the conventional liquid obtained by cooling the melt. The dependence of the transformation rate on the film thickness is consistent with a growth front mechanism for the direct conversion from the ultrastable glass to the equilibrium supercooled liquid. We conclude that the IMC liquid recovered from the ultrastable glass is structurally and dynamically identical to the conventional supercooled state.