Bilayer-folded lamellar mesophase induced by random polymer sequence

Minjoong Shin, Hayeon Kim, Geonhyeong Park, Jongmin Park, Hyungju Ahn, Dong Ki Yoon, Eunji Lee and Myungeun Seo ()
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Minjoong Shin: Korea Advanced Institute of Science and Technology (KAIST)
Hayeon Kim: Gwangju Institute of Science and Technology (GIST)
Geonhyeong Park: Korea Advanced Institute of Science and Technology (KAIST)
Jongmin Park: Korea Advanced Institute of Science and Technology (KAIST)
Hyungju Ahn: Pohang Accelerator Laboratory (PAL)
Dong Ki Yoon: Korea Advanced Institute of Science and Technology (KAIST)
Eunji Lee: Gwangju Institute of Science and Technology (GIST)
Myungeun Seo: Korea Advanced Institute of Science and Technology (KAIST)

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract Randomness is perceived in two different extremes, in macroscopic homogeneity and local heterogeneity, but apparently far away from order. Here we show that a periodic order spontaneously arises from a binary random copolymer when self-assembly occurs in an ensemble containing > 1015 possible chain sequences. A Bernoullian distribution of hydrophilic and hydrophobic side chains grafted onto a linear backbone was constructed by random copolymerization. When the polymer chains associate in water, a sequence matching problem occurs because of the drastic heterogeneity in sequence: this is believed to generate local curvature mismatches which deviate from the ensemble-averaged interfacial curvature. Periodic folding of the self-assembled bilayer stabilizes the curvature instability as recurring hinges. Reminiscent of chain-folded lamellae found in polymer crystallization, this new liquid crystalline mesophase, characterized as bilayer-folded lamellae, manifests itself as an anisotropically alignable birefringent hydrogel with structural hierarchy across multiple length scales.

Date: 2022
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DOI: 10.1038/s41467-022-30122-z

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