Polymer Glass Formation: Role of Activation Free Energy, Configurational Entropy, and Collective Motion

We provide a perspective on polymer glass formation, with an emphasis models in which the fluid entropy and collective particle motion dominate theoretical description data analysis. The theory of formation has its origins experimental observations relating to correlations between liquid dynamics going back nearly century ago, it entered new phase recent years. first discuss liquids high-temperature Arrhenius regime, where transition state is formally applicable. then summarize evolution from qualitative framework for organizing interpreting temperature-dependent viscosity by Kauzmann formulation hypothetical “ideal thermodynamic transition” Gibbs DiMarzio, followed seminal measurements linking relaxation Bestul Chang Adam–Gibbs (AG) model rationalizing Chang. These developments laid groundwork generalized (GET), merges improved lattice thermodynamics accounting molecular structural details enabling analytic calculation configurational AG model, giving rise highly predictive segmental time polymeric glass-forming liquids. development GET occurred parallel string concrete realizations cooperatively rearranging regions are identified quantified wide range other materials. shown that many assumptions well supported simulations, while others certainly not, largely accord GET. As continue be refined, these progressively grow into more unified framework, this Perspective reviews present status promising approach