Nonlinear dielectric response and thermodynamic heterogeneity in liquids

If large amplitude time-dependent fields (e.g., dielectric, magnetic, mechanical) are applied to a sample that displays relaxational modes, some energy of the external field is absorbed by the slow degrees of freedom. The weak coupling of these modes to the phonon bath leads to long persistence times of the resulting higher fictive temperature. Assuming heterogeneities regarding dielectric and thermal relaxation times, extremely strong nonlinear dielectric effects are predicted and experimentally verified. For glycerol at T = 213 K, the dielectric loss measured at 280 kV/cm increases by more than 6% over its low-field value. This nonlinearity shows a characteristic frequency dependence and implies that dielectric and thermal time constants are locally correlated in viscous liquids.