Journal
ACS NANO
Volume 8, Issue 11, Pages 11674-11684Publisher
AMER CHEMICAL SOC
DOI: 10.1021/nn505007u
Keywords
two-dimensional materials; supramolecular assembly; protein-mimetic materials; coarse-grained modeling; bioinspired polymers; interfacial assembly; monolayer compression
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Funding
- Defense Threat Reduction Agency [IACRO-B1144571]
- Advanced Light Source
- National Energy Research Scientific Computing Center, at Lawrence Berkeley National Laboratory
- Office of Science, Office of Basic Energy Sciences, U.S. Department of Energy [DE-AC02-05CH11231]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
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Organic two-dimensional nanomaterials are of growing importance, yet few general synthetic methods exist to produce them in high yields and to precisely functionalize them. We previously developed an efficient hierarchical supramolecular assembly route to peptoid bilayer nanosheets, where the organization of biomimetic polymer sequences is catalyzed by an airwater interface. Here we determine at which stages of assembly the nanoscale and atomic-scale order appear. We used X-ray scattering, grazing incidence X-ray scattering at the airwater interface, electron diffraction, and a recently developed computational coarse-grained peptoid model to probe the molecular ordering at various stages of assembly. We found that lateral packing and organization of the chains occurs during the formation of a peptoid monolayer, prior to its collapse into a bilayer. Identifying the structure-determining step enables strategies to influence nanosheet order, to predict and optimize production yields, and to further engineer this class of material. More generally, our results provide a guide for using fluid interfaces to catalytically assemble 2D nanomaterials.
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