Publications by authors named "U Buchenau"

The shear misfit model for highly viscous flow is based upon a theoretical prediction for its terminal stage in terms of irreversible Eshelby relaxations in five-dimensional shear space. The model is shown to predict a small δ-function (Debye peak) in the dielectric spectrum, in agreement with experimental evidence. It is extended to density fluctuations, and a relation between adiabatic and isothermal compressibility jumps at the glass transition is derived.

View Article and Find Full Text PDF

A recent description of the highly viscous flow ascribes it to irreversible thermally activated Eshelby transitions, which transform a region of the undercooled liquid to a different structure with a different elastic misfit to the viscoelastic surroundings. The description is extended to include reversible Eshelby transitions, with the Kohlrausch exponent β as a free parameter. The model answers several open questions in the field.

View Article and Find Full Text PDF

The highly viscous flow is due to thermally activated Eshelby transitions which transform a region of the undercooled liquid to a different structure with a different elastic misfit to the viscoelastic surroundings. A self-consistent determination of the viscosity in this picture explains why the average structural relaxation time is a factor of eight longer than the Maxwell time. The physical reason for the short Maxwell time is the very large contribution of strongly strained inherent states to the fluidity (the inverse viscosity).

View Article and Find Full Text PDF

The paper derives a relation for the viscosity of undercooled liquids on the basis of the pragmatical model concept of Eshelby relaxations with a finite lifetime. From accurate shear relaxation data in the literature, one finds that slightly less than half of the internal stresses relax directly via single Eshelby relaxations; the larger part dissolves at the terminal lifetime, which is a combined effect of many Eshelby relaxations.

View Article and Find Full Text PDF

The recently developed pragmatical model of asymmetric double-well potentials with a finite lifetime is applied to nonlinear dielectric data in polar undercooled liquids. The viscous effects from the finite lifetime provide a crossover from the cooperative jumps of many molecules at short times to the motion of statistically independent molecules at long times. The model allows us to determine the size of cooperatively rearranging regions from nonlinear ω-data and throws new light on a known inconsistency between nonlinear ω and 3ω-signals for glycerol and propylene carbonate.

View Article and Find Full Text PDF