Related papers: Generalized entropy theory of glass-formation in f…
Chemical structure has been long recognized to greatly influence polymer glass formation, but a general molecular theory that predicts how chemical structure determines the properties of glass-forming polymers has been slow to develop.…
We utilize the generalized entropy theory (GET) of glass formation to address one of the most singular and least understood properties of polymer glass-forming liquids in comparison to atomic and small molecule liquids -- the often…
We provide a perspective on polymer glass formation, with an emphasis on models in which the fluid entropy and collective particle motion dominate the theoretical description and data analysis. We first discuss the dynamics of liquids in…
Many glass-forming fluids exhibit a remarkable thermodynamic scaling in which dynamic properties, such as the viscosity, the relaxation time, and the diffusion constant, can be described under different thermodynamic conditions in terms of…
We utilize the lattice cluster theory (LCT) of polymer fluids to show that the configurational entropy, enthalpy, and internal energy are all closely interrelated, as suggested by recent measurements by Caruthers and Medvedev, so that the…
An analysis of glass formation for polymer melts that are diluted by structured molecular additives is derived by using the generalized entropy theory, which involves a combination of the Adam-Gibbs model and the direct computation of the…
We show that thermodynamic scaling can be derived by combining the Murnaghan equation of state (EOS) with the generalized entropy theory (GET) of glass formation. In our theory, thermodynamic scaling arises in the non-Arrhenius relaxation…
The generalized entropy theory is applied to assess the joint influence of the microscopic cohesive energy and chain stiffness on glass formation in polymer melts using a minimal model containing a single bending energy and a single…
We explore the nature of glass-formation in variable spatial dimensionality ($d$) based on the generalized entropy theory, a synthesis of the Adam-Gibbs model with direct computation of the configurational entropy of polymer fluids using an…
We introduce a new quantity to probe the glass transition. This quantity is a linear generalized compressibility which depends solely on the positions of the particles. We have performed a molecular dynamics simulation on a glass forming…
An extended Molecular-Dynamics study of the short-time "glassy" elasticity exhibited by a polymer melt of linear fully-flexible chains above the glass transition is presented. The focus is on the infinite-frequency shear modulus $G_\infty$…
To study the cooling behavior and the glass transition of polymer melts in bulk and with free surfaces a coarse-grained weakly semi-flexible polymer model is developed. Based on a standard bead spring model with purely repulsive…
The lattice cluster theory (LCT) for semiflexible linear telechelic melts, developed in paper I, is applied to examine the influence of chain stiffness on the average degree of self-assembly and the basic thermodynamic properties of linear…
We have connected the dynamic fragility, namely the rapidity of the relaxation time increase upon temperature reduction, to the excess entropy and heat capacity of a large number of glass-forming polymers. The connection was obtained in a…
A model of low-temperature polar liquids is constructed that accounts for configurational heat capacity, entropy, and the effect of a strong electric field on the glass transition. The model is based on Pad{\'e}-truncated perturbation…
We present Molecular Dynamics simulations of the thermal glass transition in a dense model polymer liquid. We performed a comparative study of both constant volume and constant pressure cooling of the polymer melt. Great emphasis was laid…
Understanding the nature of glass transition, as well as precise estimation of the glass transition temperature for polymeric materials, remain open questions in both experimental and theoretical polymer sciences. We propose a data-driven…
Understanding and predicting the glassy dynamics of polymers remain fundamental challenges in soft matter physics. While the Elastically Collective Nonlinear Langevin Equation (ECNLE) theory has been successful in describing relaxation…
A glass is a non-equilibrium thermodynamic state whose physical properties depend on time. Glass formation from the melt, as well as the inverse process of liquid structural recovery from the glass are non-equilibrium processes. A positive…
We propose a computational method to measure the configurational entropy in generic polydisperse glass-formers. In particular, our method resolves issues related to the diverging mixing entropy term due to a continuous polydispersity. The…