Dipole-dipole correlations and the Debye process in the dielectric response of nonassociating glass forming liquids.

Abstract

The nonexponential shape of the α process observed in supercooled liquids is considered as one of the hallmarks of glassy dynamics and has thus been under study for decades, but is still poorly understood. For a polar van der Waals liquid, we show here-in line with a recent theory-that dipole-dipole correlations give rise to an additional process in the dielectric spectrum slightly slower than the α relaxation, which renders the resulting combined peak narrower than observed by other experimental techniques. This is reminiscent of the Debye-process found in monohydroxy alcohols. The additional peak can be suppressed by weakening the dipole-dipole interaction via dilution with a nonpolar solvent.