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• W2559595705 abstract "The glass transition region in nonconfined polymeric and low-molecular-weight supercooled liquids is probed by temperature-modulated calorimetry at a frequency of 3.3 mHz. From the distribution of relaxation times derived by analyzing the complex heat capacity, the number ${N}_{ensuremath{alpha}}$ of cooperatively rearranging units is estimated. This is done by resorting to a method in which cooperative motion is viewed as a result of a spontaneous regression of energy fluctuations. After a first, local, structural transition occurs, the energy threshold for the rearrangement of adjacent molecular units decreases progressively. This facilitation process is associated to a corresponding evolution of the density of states in a canonical representation and may be considered as a continuous spanning through different dynamic states toward a condition in which configurational constraints disappear. A good agreement is found with the ${N}_{ensuremath{alpha}}$ values obtained from the same calorimetric data within the framework of Donth's fluctuation theory. It is shown that, at variance from previous treatments, ${N}_{ensuremath{alpha}}$ can be estimated from just the relaxation function, without resorting to the knowledge of the configurational entropy. Examples point to a modest dependence of the ${N}_{ensuremath{alpha}}$ estimates on the experimental method used to derive the relaxation function." @default.
• W2559595705 created "2016-12-08" @default.
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• W2559595705 date "2016-11-28" @default.
• W2559595705 modified "2023-09-26" @default.
• W2559595705 title "Cooperativity at the glass transition: A perspective from facilitation on the analysis of relaxation in modulated calorimetry" @default.
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• W2559595705 doi "https://doi.org/10.1103/physreve.94.052504" @default.
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