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Title: Reversible self-assembly of superstructured networks

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.
Authors:
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Publication Date:
Grant/Contract Number:
FG02-00ER45810; SC0000989; 2014 BP-A 00007
Type:
Published Article
Journal Name:
Science
Additional Journal Information:
Journal Name: Science Journal Volume: 362 Journal Issue: 6416; Journal ID: ISSN 0036-8075
Publisher:
American Association for the Advancement of Science (AAAS)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
OSTI Identifier:
1482288

Freeman, Ronit, Han, Ming, Álvarez, Zaida, Lewis, Jacob A., Wester, James R., Stephanopoulos, Nicholas, McClendon, Mark T., Lynsky, Cheyenne, Godbe, Jacqueline M., Sangji, Hussain, Luijten, Erik, and Stupp, Samuel I.. Reversible self-assembly of superstructured networks. United States: N. p., Web. doi:10.1126/science.aat6141.
Freeman, Ronit, Han, Ming, Álvarez, Zaida, Lewis, Jacob A., Wester, James R., Stephanopoulos, Nicholas, McClendon, Mark T., Lynsky, Cheyenne, Godbe, Jacqueline M., Sangji, Hussain, Luijten, Erik, & Stupp, Samuel I.. Reversible self-assembly of superstructured networks. United States. doi:10.1126/science.aat6141.
Freeman, Ronit, Han, Ming, Álvarez, Zaida, Lewis, Jacob A., Wester, James R., Stephanopoulos, Nicholas, McClendon, Mark T., Lynsky, Cheyenne, Godbe, Jacqueline M., Sangji, Hussain, Luijten, Erik, and Stupp, Samuel I.. 2018. "Reversible self-assembly of superstructured networks". United States. doi:10.1126/science.aat6141.
@article{osti_1482288,
title = {Reversible self-assembly of superstructured networks},
author = {Freeman, Ronit and Han, Ming and Álvarez, Zaida and Lewis, Jacob A. and Wester, James R. and Stephanopoulos, Nicholas and McClendon, Mark T. and Lynsky, Cheyenne and Godbe, Jacqueline M. and Sangji, Hussain and Luijten, Erik and Stupp, Samuel I.},
abstractNote = {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.},
doi = {10.1126/science.aat6141},
journal = {Science},
number = 6416,
volume = 362,
place = {United States},
year = {2018},
month = {10}
}

Works referenced in this record:

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