A two-fluid model for the formation of clusters close to a continuous or almost continuous transition View Full Text


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Article Info

DATE

2021-09-02

AUTHORS

Harald Pleiner, Helmut R. Brand

ABSTRACT

Experiments have shown that spatial heterogeneities can arise when the glass transition in polymers as well as in a number of low molecular weight compounds is approached by lowering the temperature. This formation of “clusters” has been detected predominantly by small angle light scattering and ultrasmall angle x-ray scattering from the central peak on length scales up to about 200 nm and by mechanical measurements including, in particular, piezorheometry for length scales up to several microns. Here we use a macroscopic two-fluid model to study the formation of clusters observed by the various experimental techniques. As additional macroscopic variables, when compared to simple fluids, we use a transient strain field to incorporate transient positional order, along with the velocity difference and a relaxing concentration field for the two subsystems. We show that an external homogeneous shear, as it is applied in piezorheometry, can lead to the onset of spatial pattern formation. To address the issue of additional spectral weight under the central peak we investigate the coupling to all macroscopic variables. We find that there are additional static as well as dissipative contributions from both, transient positional order, as well as from concentration variations due to cluster formation, and additional reversible couplings from the velocity difference. We also briefly discuss the influence of transient orientational order. Finally, we point out that our description is more general, and could be applied above continuous or almost continuous transitions More... »

PAGES

675-690

References to SciGraph publications

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  • 2016-07. Peculiarities of light scattering by boron oxide glass in GLASS PHYSICS AND CHEMISTRY
  • 2002-01. Convective nonlinearities for the orientational tensor order parameter in polymeric systems in RHEOLOGICA ACTA
  • 2009-12. Disordered, quasicrystalline and crystalline phases of densely packed tetrahedra in NATURE
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  • 2018-10-05. Dissipative versus reversible contributions to macroscopic dynamics: the role of time-reversal symmetry and entropy production in RHEOLOGICA ACTA
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    http://scigraph.springernature.com/pub.10.1007/s00397-021-01296-y

    DOI

    http://dx.doi.org/10.1007/s00397-021-01296-y

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