Nanopatterned Monolayers of Bioinspired, Sequence-Defined Polypeptoid Brushes for Semiconductor/Bio Interfaces
Abstract
The ability to control and manipulate semiconductor/bio interfaces is essential to enable biological nanofabrication pathways and bioelectronic devices. Traditional surface functionalization methods, such as self-assembled monolayers (SAMs), provide limited customization for these interfaces. Polymer brushes offer a wider range of chemistries, but choices that maintain compatibility with both lithographic patterning and biological systems are scarce. Here, we developed a class of bioinspired, sequence-defined polymers, i.e., polypeptoids, as tailored polymer brushes for surface modification of semiconductor substrates. Polypeptoids featuring a terminal hydroxyl (–OH) group are designed and synthesized for efficient melt grafting onto the native oxide layer of Si substrates, forming ultrathin (~1 nm) monolayers. By programming monomer chemistry, our polypeptoid brush platform offers versatile surface modification, including adjustments to surface energy, passivation, preferential biomolecule attachment, and specific biomolecule binding. Importantly, the polypeptoid brush monolayers remain compatible with electron-beam lithographic patterning and retain their chemical characteristics even under harsh lithographic conditions. Electron-beam lithography is used over polypeptoid brushes to generate highly precise, binary nanoscale patterns with localized functionality for the selective immobilization (or passivation) of biomacromolecules, such as DNA origami or streptavidin, onto addressable arrays. This surface modification strategy with bioinspired, sequence-defined polypeptoid brushes enables monomer-level control over surface properties withmore »
- Authors:
-
- The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
- The Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States, Prizker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60637, United States
- Molecular Vista Inc., San Jose, California 95119, United States
- Department of Electrical Engineering and Computer Sciences, University of California, Berkeley, Berkeley, California 94709, United States
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Laboratory Directed Research and Development (LDRD) Program
- OSTI Identifier:
- 2315050
- Alternate Identifier(s):
- OSTI ID: 2323240
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Published Article
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Name: ACS Nano Journal Volume: 18 Journal Issue: 10; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; nanopatterned polymer brushes; sequence-defined polymers; semiconductor/bio interfaces; surface modification; selective immobilization of biomolecules
Citation Formats
Yu, Beihang, Chang, Boyce S., Loo, Whitney S., Dhuey, Scott, O’Reilly, Padraic, Ashby, Paul D., Connolly, Michael D., Tikhomirov, Grigory, Zuckermann, Ronald N., and Ruiz, Ricardo. Nanopatterned Monolayers of Bioinspired, Sequence-Defined Polypeptoid Brushes for Semiconductor/Bio Interfaces. United States: N. p., 2024.
Web. doi:10.1021/acsnano.3c10204.
Yu, Beihang, Chang, Boyce S., Loo, Whitney S., Dhuey, Scott, O’Reilly, Padraic, Ashby, Paul D., Connolly, Michael D., Tikhomirov, Grigory, Zuckermann, Ronald N., & Ruiz, Ricardo. Nanopatterned Monolayers of Bioinspired, Sequence-Defined Polypeptoid Brushes for Semiconductor/Bio Interfaces. United States. https://doi.org/10.1021/acsnano.3c10204
Yu, Beihang, Chang, Boyce S., Loo, Whitney S., Dhuey, Scott, O’Reilly, Padraic, Ashby, Paul D., Connolly, Michael D., Tikhomirov, Grigory, Zuckermann, Ronald N., and Ruiz, Ricardo. Tue .
"Nanopatterned Monolayers of Bioinspired, Sequence-Defined Polypeptoid Brushes for Semiconductor/Bio Interfaces". United States. https://doi.org/10.1021/acsnano.3c10204.
@article{osti_2315050,
title = {Nanopatterned Monolayers of Bioinspired, Sequence-Defined Polypeptoid Brushes for Semiconductor/Bio Interfaces},
author = {Yu, Beihang and Chang, Boyce S. and Loo, Whitney S. and Dhuey, Scott and O’Reilly, Padraic and Ashby, Paul D. and Connolly, Michael D. and Tikhomirov, Grigory and Zuckermann, Ronald N. and Ruiz, Ricardo},
abstractNote = {The ability to control and manipulate semiconductor/bio interfaces is essential to enable biological nanofabrication pathways and bioelectronic devices. Traditional surface functionalization methods, such as self-assembled monolayers (SAMs), provide limited customization for these interfaces. Polymer brushes offer a wider range of chemistries, but choices that maintain compatibility with both lithographic patterning and biological systems are scarce. Here, we developed a class of bioinspired, sequence-defined polymers, i.e., polypeptoids, as tailored polymer brushes for surface modification of semiconductor substrates. Polypeptoids featuring a terminal hydroxyl (–OH) group are designed and synthesized for efficient melt grafting onto the native oxide layer of Si substrates, forming ultrathin (~1 nm) monolayers. By programming monomer chemistry, our polypeptoid brush platform offers versatile surface modification, including adjustments to surface energy, passivation, preferential biomolecule attachment, and specific biomolecule binding. Importantly, the polypeptoid brush monolayers remain compatible with electron-beam lithographic patterning and retain their chemical characteristics even under harsh lithographic conditions. Electron-beam lithography is used over polypeptoid brushes to generate highly precise, binary nanoscale patterns with localized functionality for the selective immobilization (or passivation) of biomacromolecules, such as DNA origami or streptavidin, onto addressable arrays. This surface modification strategy with bioinspired, sequence-defined polypeptoid brushes enables monomer-level control over surface properties with a large parameter space of monomer chemistry and sequence and therefore is a highly versatile platform to precisely engineer semiconductor/bio interfaces for bioelectronics applications.},
doi = {10.1021/acsnano.3c10204},
journal = {ACS Nano},
number = 10,
volume = 18,
place = {United States},
year = {Tue Feb 27 00:00:00 EST 2024},
month = {Tue Feb 27 00:00:00 EST 2024}
}
https://doi.org/10.1021/acsnano.3c10204
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