4.7 Article

Susceptibility functions for slow relaxation processes in supercooled liquids and the search for universal relaxation patterns

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JOURNAL OF CHEMICAL PHYSICS
卷 118, 期 16, 页码 7544-7555

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AMER INST PHYSICS
DOI: 10.1063/1.1563247

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In order to describe the slow response of a glass former, we discuss some distributions of correlation times, e.g., a generalized gamma distribution (GG) and an extension thereof (GGE), the latter allowing us to reproduce a simple peak susceptibility such as of the Cole-Davidson type as well as a susceptibility exhibiting an additional high-frequency power law contribution (excess wing). Applying the GGE distribution to the dielectric spectra of glass formers exhibiting no beta process peak (glycerol, propylene carbonate, and picoline) we are able to reproduce the salient features of the slow response (10(-6)-10(9) Hz). A line shape analysis is carried out either in the time or frequency domain and in both cases an excess wing can be identified. The latter evolves in a universal way while cooling and shows up for correlation times tau(alpha)>10(-8) s. It appears that its first emergence marks the breakdown of the high-temperature scenario of mode coupling theory. In order to describe a glass former exhibiting a beta process peak we have introduced a distribution function which is compatible with assuming a thermally activated process in contrast to some commonly used fit functions. Together with the GGE distribution this function allows in the frame of the Williams-Watts approach to completely interpolate the spectra, e.g., of fluoro aniline (10(-6) Hz-10(9) Hz). The parameters obtained indicate an emergence of both the excess wing and the beta process again at tau(alpha)>10(-8) s. (C) 2003 American Institute of Physics.

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