Dynamic Heterogeneity and Cooperative Length Scale at Dynamic Glass Transition in Glass Forming Liquids

• Published in: Macromolecules 2015-11, Vol.48 (22), p.8219-8231
• Main Authors: Rijal, Bidur, Delbreilh, Laurent, Saiter, Allisson
• Format: Article
• Language: English
• Subjects: Condensed Matter; Materials Science; Physics
• ISSN: 0024-9297; 1520-5835
• DOI: 10.1021/acs.macromol.5b01152

Understanding the evolution of the cooperative molecular mobility as a function of time and temperature remains an unsolved question in condensed matter research. However, recently great advances have been made within the framework of the Adam–Gibbs theory on the connection between cooperatively rearranging regions, or dynamic heterogeneities, i.e., domains of the supercooled liquid whose relaxation is highly correlated. The growth of the size of these dynamic domains is now believed to be the driving mechanism for different experimental parameters like relaxation times and viscosity of supercooled liquid approaching the glass transition. Recent studies have shown the evolution of cooperative motions in supercooled liquids using different experimental tools and models. In this work, broadband dielectric spectroscopy and modulated temperature differential scanning calorimetry were carried out on six different amorphous glass-forming systems in order to scan a wide range of relaxation times and temperatures. Two different models based on four point dynamic susceptibilities and the thermodynamic fluctuation approach, have been used to compare the temperature evolution of the number of molecules dynamically correlated during the α-relaxation process. Divergences and convergences between these two models are discussed.