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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 α 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 α …
American Physical Society
Publication date: 
28 Nov 2016

Elpidio Tombari, Marco Pieruccini

Biblio References: 
Volume: 94 Issue: 5 Pages: 052504
Physical Review E