Elastic models for the non-Arrhenius viscosity of glass-forming liquids

This paper first reviews the shoving model for the non-Arrhenius viscosity of viscous liquids. According to this model the main contribution to the activation energy of a flow event is the energy needed for molecules to shove aside the surrounding, an energy which is proportional to the instantaneous shear modulus of the liquid. Data are presented supporting the model. It is shown that the fractional Debye-Stokes-Einstein relation, that quantitatively expresses the frequently observed decoupling of, e.g., conductivity from viscous flow, may be understood within the model. The paper goes on to review several related explanations for the non-Arrhenius viscosity. Most of these are also "elastic models," i.e., they express the viscosity activation energy in terms of short-time elastic properties of the liquid. Finally, two new arguments for elastic models are given, a general solid-state defect argument and an Occam's razor type argument

Beta relaxation in the shear mechanics of equilibrium viscous liquids: Phenomenology and network modeling of the alpha-beta merging region

The phenomenology of the beta relaxation process in the shear-mechanical response of glass-forming liquids is summarized and compared to that of the dielectric beta process. Furthermore, we discuss how to model the observations by means of standard viscoelastic modeling elements. Necessary physical requirements to such a model are outlined, and it is argued that physically relevant models must be additive in the shear compliance of the alpha and beta parts. A model based on these considerations is proposed and fitted to data for Polyisobutylene 680.Comment: 8 pages, 6 figures, Minor correction

The mixed convolved action

A series of stationary principles are developed for dynamical systems by formulating the concept of mixed convolved action, which is written in terms of mixed variables, using temporal convolutions and fractional derivatives. Dynamical systems with discrete and continuous spatial representations are considered as initial applications. In each case, a single scalar functional provides the governing differential equations, along with all the pertinent initial and boundary conditions, as the Euler-Lagrange equations emanating from the stationarity of this mixed convolved action. Both conservative and non-conservative processes can be considered within a common framework, thus resolving a long-standing limitation of variational approaches for dynamical systems. Several results in fractional calculus also are developed

Dielectric and thermal relaxation in the energy landscape

We derive an energy landscape interpretation of dielectric relaxation times in undercooled liquids, comparing it to the traditional Debye and Gemant-DiMarzio-Bishop pictures. The interaction between different local structural rearrangements in the energy landscape explains qualitatively the recently observed splitting of the flow process into an initial and a final stage. The initial mechanical relaxation stage is attributed to hopping processes, the final thermal or structural relaxation stage to the decay of the local double-well potentials. The energy landscape concept provides an explanation for the equality of thermal and dielectric relaxation times. The equality itself is once more demonstrated on the basis of literature data for salol.Comment: 7 pages, 3 figures, 41 references, Workshop Disordered Systems, Molveno 2006, submitted to Philosophical Magazin