title: Electrostatic control of structure in self-assembled membranes.
abstract: Self-assembling peptide amphiphiles (PAs) can form hierarchically ordered membranes when brought in contact with aqueous polyelectrolytes of the opposite charge by rapidly creating a diffusion barrier composed of filamentous nanostructures parallel to the plane of the incipient membrane. Following this event, osmotic forces and charge complexation template nanofiber growth perpendicular to the plane of the membrane in a dynamic self-assembly process. In this work, we show that this hierarchical structure requires massive interfacial aggregation of PA molecules, suggesting the importance of rapid diffusion barrier formation. Strong PA aggregation is induced here through the use of heparin-binding PAs with heparin and also with polyelectrolytes of varying charge density. Small angle X-ray scattering shows that in the case of weak PA-polyelectrolyte interaction, membranes formed display a cubic phase ordering on the nanoscale that likely results from clusters of PA nanostructures surrounded by polyelectrolyte chains.
authors.affiliation: Institute for BioNanotechnology in Medicine, Northwestern University, Chicago, IL, 60611, USA.
authors.forename: Ronit
authors.initials: R
authors.lastname: Bitton
authors.forename: Lesley W
authors.initials: LW
authors.lastname: Chow
authors.forename: R Helen
authors.initials: RH
authors.lastname: Zha
authors.forename: Yuri S
authors.initials: YS
authors.lastname: Velichko
authors.forename: E Thomas
authors.initials: ET
authors.lastname: Pashuck
authors.forename: Samuel I
authors.initials: SI
authors.lastname: Stupp
mesh_terms: D000180:Acrylic Resins / Q000737:chemistry; D000464:Alginates / Q000737:chemistry; D023181:Antimicrobial Cationic Peptides / Q000737:chemistry; D001798:Blood Proteins / Q000737:chemistry; D002351:Carrageenan / Q000737:chemistry; D002352:Carrier Proteins / Q000737:chemistry; D020723:Glucuronic Acid / Q000737:chemistry; D006603:Hexuronic Acids / Q000737:chemistry; D006820:Hyaluronic Acid / Q000737:chemistry; D008567:Membranes, Artificial; D008855:Microscopy, Electron, Scanning; D049329:Nanostructures / Q000648:ultrastructure; D010455:Peptides / Q000737:chemistry; D053838:Scattering, Small Angle; D055672:Static Electricity; D013501:Surface-Active Agents / Q000737:chemistry; D014961:X-Ray Diffraction
chemical_list: C062991:AZU1 protein, human; D000180:Acrylic Resins; D000464:Alginates; D023181:Antimicrobial Cationic Peptides; D001798:Blood Proteins; D002352:Carrier Proteins; D006603:Hexuronic Acids; D008567:Membranes, Artificial; D010455:Peptides; D013501:Surface-Active Agents; C006903:carbopol 940; D020723:Glucuronic Acid; D002351:Carrageenan; D006820:Hyaluronic Acid
keywords: SAXS; ordered membranes; peptide amphiphiles; polyelectrolyte-supramolecular polymer complex; self-assembly
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