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  • Title: The dynamic susceptibility in glass forming molecular liquids: the search for universal relaxation patterns II.
    Author: Blochowicz T, Gainaru C, Medick P, Tschirwitz C, Rössler EA.
    Journal: J Chem Phys; 2006 Apr 07; 124(13):134503. PubMed ID: 16613457.
    Abstract:
    The susceptibility spectra of ten molecular glass formers are completely interpolated by an extension of the generalized gamma distribution of correlation times. The data cover at least 15 decades in frequency and the interpolation includes both alpha peak and excess wing. It is shown that the line shape parameters and the time constant of the alpha relaxation are related to each other. Master curves are identified by a scaling procedure that involves only three parameters, namely, the glass transition temperature T(g), the fragility m, and the excess wing exponent at T(g). This holds independent of whether a further secondary relaxation peak is present or not. Above a crossover temperature T(x) this unique evolution of the line shape parameters breaks down, and a crossover to a simple peak susceptibility without excess wing is observed. Here, the frequency-temperature superposition principle holds in good approximation up to temperatures well above the melting point. It turns out that the crossover coincides with the temperature at which the low-temperature Vogel-Fulcher law starts to fail upon heating. Thus, the so-called Stickel temperature gets a more physical meaning as it marks a qualitative change in the evolution of the susceptibility spectra of glass formers. Moreover, the interrelation of the line shape parameters can explain why the "Nagel scaling" works in some approximation. Our study demonstrates that the excess wing in molecular glass formers is a secondary relaxation, which is linked to the alpha process in a unique way.
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