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Stress anisotropy in polymer brushes and its effects on wetting

Lars B. VeldscholteJacco H. SnoeijerSissi de Beer
Dec 2022
摘要
Polymer brushes, coatings consisting of densely grafted macromolecules, havebeen known to experience an intrinsic lateral compressive stress, originatingfrom chain elasticity and excluded volume interactions. This lateral stresscomplicates a proper definition of the interface and, thereby, of theinterfacial tension. Moreover, its effect on wettability has remained unclear.Here, we study the link between grafting-induced compressive lateral stress inpolymer brushes, interfacial tension, and brush wettability usingcoarse-grained molecular dynamics simulations. A central result is that theliquid contact angle is independent of grafting density, which implies that thestrength of the compressive stress inside brush has no influence on thewettability. Interestingly, though the interfacial tensions lack a properdefinition, the difference in interfacial tension between wet and dry brushesis perfectly well-defined. We confirm explicitly from Young's law that thisdifference offers an accurate description of the brush wettability. It isdemonstrated how these results can be explained from the fact that thecompressive stress appears "symmetrically" in wet and dry brushes. We discussour findings in the light of autophobic dewetting and point out the connectionto the Shuttleworth effect for wetting on elastomers.
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