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Article Dans Une Revue European Physical Journal E: Soft matter and biological physics Année : 2023

On the bridge hypothesis in the glass transition of freestanding polymer films

Haggai Bonneau
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Maxence Arutkin
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Rainni Chen
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James A Forrest
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Elie Raphaël
Thomas Salez

Résumé

Freestanding thin polymer films with high molecular weights exhibit an anomalous decrease in the glass-transition temperature with film thickness. Specifically, in such materials, the measured glass-transition temperature evolves in an affine way with the film thickness, with a slope that weakly depends on the molecular weight. De Gennes proposed a sliding mechanism as the hypothetical dominant relaxation process in these systems, where stress kinks could propagate in a reptation-like fashion through so called bridges, i.e. from one free interface to the other along the backbones of polymer macromolecules. Here, by considering the exact statistics of finite-sized random walks within a confined box, we investigate in details the bridge hypothesis. We show that the sliding mechanism cannot reproduce the basic features appearing in the experiments, and we exhibit the fundamental reasons behind such a fact.
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Dates et versions

hal-03889405 , version 1 (08-12-2022)

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Citer

Haggai Bonneau, Maxence Arutkin, Rainni Chen, James A Forrest, Elie Raphaël, et al.. On the bridge hypothesis in the glass transition of freestanding polymer films. European Physical Journal E: Soft matter and biological physics, 2023, 46 (3), pp.8. ⟨10.1140/epje/s10189-023-00272-z⟩. ⟨hal-03889405⟩
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