Reversible self-assembly of superstructured networks.
Ronit FreemanMing HanZaida ÁlvarezJacob A LewisJames R WesterNicholas StephanopoulosMark T McClendonCheyenne LynskyJacqueline M GodbeM Hussain SangjiErik LuijtenSamuel I StuppPublished in: Science (New York, N.Y.) (2018)
Soft structures in nature, such as protein assemblies, can organize reversibly into functional and often hierarchical architectures through noncovalent interactions. Molecularly encoding this dynamic capability in synthetic materials has remained an elusive goal. We report on hydrogels of peptide-DNA conjugates and peptides that organize into superstructures of intertwined filaments that disassemble upon the addition of molecules or changes in charge density. Experiments and simulations demonstrate that this response requires large-scale spatial redistribution of molecules directed by strong noncovalent interactions among them. Simulations also suggest that the chemically reversible structures can only occur within a limited range of supramolecular cohesive energies. Storage moduli of the hydrogels change reversibly as superstructures form and disappear, as does the phenotype of neural cells in contact with these materials.
Keyphrases
- drug delivery
- induced apoptosis
- molecular dynamics
- hyaluronic acid
- high resolution
- drug release
- cell cycle arrest
- monte carlo
- extracellular matrix
- density functional theory
- tissue engineering
- amino acid
- circulating tumor
- wound healing
- single molecule
- cancer therapy
- cell free
- endoplasmic reticulum stress
- cell death
- oxidative stress
- binding protein
- energy transfer
- solar cells
- cell proliferation
- mass spectrometry
- circulating tumor cells
- small molecule
- water soluble
- pi k akt