Relationship between molecular structure and corrugations in self-assembled polypeptoid nanosheets revealed by cryogenic electron microscopy

Jiang, Xi; Zuckermann, Ronald N.; Balsara, Nitash P.

doi:10.1103/PhysRevMaterials.8.020301

Title: Relationship between molecular structure and corrugations in self-assembled polypeptoid nanosheets revealed by cryogenic electron microscopy

Journal Article · 12 February 2024 · Physical Review Materials

DOI: https://doi.org/10.1103/PhysRevMaterials.8.020301 · OSTI ID:2301714

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Designing conformationally dynamic molecules that self-assemble into predictable nanostructures remains an important unmet challenge. This paper describes how atomic-scale cryogenic transmission electron microscopy (cryo-TEM) can be used to explore the relationship between molecular structure and self-assembly of block copolymers. We examined sheetlike micelles formed in water using a series of diblock copolypeptoids with the same hydrophilic block and three distinct crystalline hydrophobic blocks. Our cryo-TEM images revealed all the structures share nansoscale features, but differ in their intermolecular packing geometries. Different molecular arrangements, parallel and antiparallel V-shaped crystal motifs, were revealed by two-dimensional atomic-scale through-plane images. However, images from tilted samples revealed an unexpected feature when the hydrophobic polypeptoid block comprised phenyl rings with substituted bromine atoms at the para position. The nanosheets contained atomic-scale corrugations that were absent in the other systems which comprised unsubstituted aliphatic and aromatic side chains. We hypothesize that these corrugations are due to the dipolar characteristics of the brominated phenyl group and interactions between this group and water molecules. Published by the American Physical Society 2024

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Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2301714

Alternate ID(s):: OSTI ID: 2433805

Journal Information:: Physical Review Materials, Journal Name: Physical Review Materials Journal Issue: 2 Vol. 8; ISSN PRMHAR; ISSN 2475-9953

Publisher:: American Physical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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