Manipulating the ABCs of self-assembly via low-{chi} block polymer design [Chemistry]
![Manipulating the ABCs of self-assembly via low-{chi} block polymer design [Chemistry]](/image/eyJ1cmkiOiJodHRwOi8vd3d3LnBuYXMub3JnL2NvbnRlbnQvMTE0LzI1LzY0NjIvRjEubWVkaXVtLmdpZiIsImZvcm1hdCI6IndlYnAiLCJxdWFsaXR5IjoxMDAsIm5vQ2FjaGUiOnRydWV9.webp)
Block polymer self-assembly typically translates molecular chain connectivity into mesoscale structure by exploiting incompatible
blocks with large interaction parameters (χij). In this article, we demonstrate that the converse approach, encoding low-χ interactions in ABC bottlebrush triblock terpolymers
(χAC
≲ 0), promotes organization into a unique mixed-domain lamellar morphology, which we designate LAMP. Transmission electron microscopy indicates that LAMP exhibits ACBC domain connectivity, in contrast to conventional three-domain lamellae (LAM3) with ABCB periods. Complementary small-angle X-ray scattering experiments reveal a strongly decreasing domain spacing with
increasing total molar mass. Self-consistent field theory reinforces these observations and predicts that LAMP is thermodynamically stable below a critical χAC, above which LAM3 emerges. Both experiments and theory expose close analogies to ABA′ triblock copolymer phase behavior, collectively suggesting
that low-χ interactions between chemically similar or distinct blocks intimately influence self-assembly. These conclusions
provide fresh opportunities for block polymer design with potential consequences spanning all self-assembling soft materials.
Publisher URL: http://www.pnas.org/content/114/25/6462.short
DOI: 10.1073/pnas.1701386114
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