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Title: Multivalent, multiflavored droplets by design

Abstract

Nature self-assembles functional materials by programming flexible linear arrangements of molecules and then folding them to make 2D and 3D objects. To understand and emulate this process, we have made emulsion droplets with specific recognition and controlled valence. Uniquely monovalent droplets form dimers: divalent lead to polymer-like chains, trivalent allow for branching, and programmed mixtures of different valences enable a variety of designed architectures and the ability to subsequently close and open structures. Our functional building blocks are a hybrid of micrometer-scale emulsion droplets and nanoscale DNA origami technologies. Functional DNA origami rafts are first added to droplets and then herded into a patch using specifically designated “shepherding” rafts. Additional patches with the same or different specificities can be formed on the same droplet, programming multiflavored, multivalence droplets. The mobile patch can bind to a patch on another droplet containing complementary functional rafts, leading to primary structure formation. Further binding of nonneighbor droplets can produce secondary structures, a third step in hierarchical self-assembly. As a result, the use of mobile patches rather than uniform DNA coverage has the advantage of valence control at the expense of slow kinetics. Droplets with controlled flavors and valences enable a host of different materialmore » and device architectures.« less

Authors:
; ; ; ; ; ;
Publication Date:
Research Org.:
New York Univ. (NYU), New York, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1466882
Alternate Identifier(s):
OSTI ID: 1540272
Grant/Contract Number:  
SC0007991
Resource Type:
Journal Article: Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 115 Journal Issue: 37; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; Science & Technology; Other Topics; patchy particle; self-assembly; DNA origami

Citation Formats

Zhang, Yin, He, Xiaojin, Zhuo, Rebecca, Sha, Ruojie, Brujic, Jasna, Seeman, Nadrian C., and Chaikin, Paul M. Multivalent, multiflavored droplets by design. United States: N. p., 2018. Web. doi:10.1073/pnas.1718511115.
Zhang, Yin, He, Xiaojin, Zhuo, Rebecca, Sha, Ruojie, Brujic, Jasna, Seeman, Nadrian C., & Chaikin, Paul M. Multivalent, multiflavored droplets by design. United States. doi:10.1073/pnas.1718511115.
Zhang, Yin, He, Xiaojin, Zhuo, Rebecca, Sha, Ruojie, Brujic, Jasna, Seeman, Nadrian C., and Chaikin, Paul M. Mon . "Multivalent, multiflavored droplets by design". United States. doi:10.1073/pnas.1718511115.
@article{osti_1466882,
title = {Multivalent, multiflavored droplets by design},
author = {Zhang, Yin and He, Xiaojin and Zhuo, Rebecca and Sha, Ruojie and Brujic, Jasna and Seeman, Nadrian C. and Chaikin, Paul M.},
abstractNote = {Nature self-assembles functional materials by programming flexible linear arrangements of molecules and then folding them to make 2D and 3D objects. To understand and emulate this process, we have made emulsion droplets with specific recognition and controlled valence. Uniquely monovalent droplets form dimers: divalent lead to polymer-like chains, trivalent allow for branching, and programmed mixtures of different valences enable a variety of designed architectures and the ability to subsequently close and open structures. Our functional building blocks are a hybrid of micrometer-scale emulsion droplets and nanoscale DNA origami technologies. Functional DNA origami rafts are first added to droplets and then herded into a patch using specifically designated “shepherding” rafts. Additional patches with the same or different specificities can be formed on the same droplet, programming multiflavored, multivalence droplets. The mobile patch can bind to a patch on another droplet containing complementary functional rafts, leading to primary structure formation. Further binding of nonneighbor droplets can produce secondary structures, a third step in hierarchical self-assembly. As a result, the use of mobile patches rather than uniform DNA coverage has the advantage of valence control at the expense of slow kinetics. Droplets with controlled flavors and valences enable a host of different material and device architectures.},
doi = {10.1073/pnas.1718511115},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
issn = {0027-8424},
number = 37,
volume = 115,
place = {United States},
year = {2018},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1073/pnas.1718511115

Citation Metrics:
Cited by: 2 works
Citation information provided by
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Figures / Tables:

Fig. 1 Fig. 1: Patch generation and valency control. (A) A droplet coated with complementary leg sticky ends is fabricated first. (Inset) The DNA strands are coated on the droplet surface through biotin–streptavidin–biotin linkages. The functional DNA origami rafts (FR_A in red and FR_B in green) carrying multiple singlestranded legs are thenmore » constructed, and mixed with the droplets at a ratio of 400:1. The functional rafts are anchored to the droplet surface via leg sticky-end hybridization. In the next step, an excess quantity of the shepherding rafts (SR_A in pink and SR_B in light green) carrying the same leg sticky ends are introduced and hybridized to the droplet surface gradually. Finally, the self-assembly of functional rafts and shepherding rafts via horizontal sticky-end binding leads to the patch formation (Patch_A and Patch_B). (Our patches use functional and complementary shepherding rafts added sequentially, rather than self-complementary functional rafts alone, to avoid patch formation in the solution.) (B) Schematics of functional and shepherding DNA origami rafts. Both rafts are decorated with six single-stranded extensions (leg sticky ends, yellow curls) on the bottom face. The two horizontal sticky-end sets (red and purple curls) on the functional raft are complementary to the two sets (pink and light purple curls) on the shepherding raft. The eight biotinylated staples (green dots) extruding from the top of the functional raft bind to the fluorescent streptavidin (red quatrefoil, for patch imaging) conjugated with arm sticky ends (blue curls, for patch functionalization). (C) AFM image of functional DNA origami rafts. (D) AFM image of shepherding DNA origami rafts. (Scale bars, 100 nm.)« less

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