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The new insight into dynamic crossover in glass forming liquids from the apparent enthalpy analysis
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/content/aip/journal/jcp/137/6/10.1063/1.4739750
2012-08-08
2014-08-22

Abstract

One of the most intriguing phenomena in glass forming systems is the dynamic crossover (T B ), occurring well above the glass temperature (T g ). So far, it was estimated mainly from the linearized derivative analysis of the primary relaxation time τ(T) or viscosity η(T) experimental data, originally proposed by Stickel et al. [J. Chem. Phys.104, 2043 (1996)10.1063/1.470961; Stickel et al.J. Chem. Phys.107, 1086 (1997)]10.1063/1.474456. However, this formal procedure is based on the general validity of the Vogel-Fulcher-Tammann equation, which has been strongly questioned recently [T. Hecksher et al.Nature Phys.4, 737 (2008)10.1038/nphys1033; P. Lunkenheimer et al.Phys. Rev. E81, 051504 (2010)10.1103/PhysRevE.81.051504; J. C. Martinez-Garcia et al.J. Chem. Phys.134, 024512 (2011)]10.1063/1.3514589. We present a qualitatively new way to identify the dynamic crossover based on the apparent enthalpy space () analysis via a new plot vs. 1/T supported by the Savitzky-Golay filtering procedure for getting an insight into the noise-distorted high order derivatives. It is shown that depending on the ratio between the “virtual” fragility in the high temperature dynamic domain (m high ) and the “real” fragility at T g (the low temperature dynamic domain, m = m low ) glass formers can be splitted into two groups related to f < 1 and f > 1, (f = m high /m low ). The link of this phenomenon to the ratio between the apparent enthalpy and activation energy as well as the behavior of the configurational entropy is indicated.

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Scitation: The new insight into dynamic crossover in glass forming liquids from the apparent enthalpy analysis
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