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Download Hi-Res ImageDownload to MS-PowerPointCite This:ACS Macro Lett. 2018, 7, 3, 281-286
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Synthesis and Direct Observation of Thermoresponsive DNA Copolymers

  • Songsong Li
    Songsong Li
    Department of Materials Science and Engineering, University of Illinois at Urbana—Champaign, Urbana, Illinois 61801, United States
    More by Songsong Li
  •  and 
  • Charles M. Schroeder*
    Charles M. Schroeder
    Department of Materials Science and Engineering, University of Illinois at Urbana—Champaign, Urbana, Illinois 61801, United States
    Department of Chemical and Biomolecular Engineering, University of Illinois at Urbana—Champaign, Urbana, Illinois 61801, United States
    *E-mail: [email protected]
    More by Charles M. Schroeder
    Orcidhttp://orcid.org/0000-0001-6023-2274
Cite this: ACS Macro Lett. 2018, 7, 3, 281–286
Publication Date (Web):February 14, 2018
https://doi.org/10.1021/acsmacrolett.8b00016
Copyright © 2018 American Chemical Society
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    Abstract

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    Single-molecule techniques allow for the direct observation of long-chain macromolecules, and these methods can provide a molecular understanding of chemically heterogeneous and stimuli-response polymers. In this work, we report the synthesis and direct observation of thermoresponsive DNA copolymers using single-molecule techniques. DNA-PNIPAM copolymers are synthesized using a two-step strategy based on polymerase chain reaction (PCR) for generating linear DNA backbones containing non-natural nucleotides (dibenzocyclooctyne-dUTP), followed by grafting thermoresponsive side branches (poly(N-isopropylacrylamide), PNIPAM) onto DNA backbones using copper-free click chemistry. Single-molecule fluorescence microscopy is used to directly observe the stretching and relaxation dynamics of DNA-PNIPAM copolymers both below and above the lower critical solution temperature (LCST) of PNIPAM. Our results show that the intramolecular conformational dynamics of DNA-PNIPAM copolymers are affected by temperature, branch density, and branch molecular weight. Single-molecule experiments reveal an underlying molecular heterogeneity associated with polymer stretching and relaxation behavior, which arises in part due to heterogeneous chemical identity on DNA copolymer dynamics.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsmacrolett.8b00016.

    • Details of DNA-PNIPAM polymer synthesis, microdevice fabrication, surface preparation, and single-molecule imaging (PDF)

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    Cited By

    This article is cited by 10 publications.

    1. Donggeng Yu, Antonio Garcia IV, Suzanne A. Blum, Kevin D. Welsher. Growth Kinetics of Single Polymer Particles in Solution via Active-Feedback 3D Tracking. Journal of the American Chemical Society 2022, 144 (32) , 14698-14705. https://doi.org/10.1021/jacs.2c04990
    2. Yu Song, Ziwen Ma, Wenke Zhang. Manipulation of a Single Polymer Chain: From the Nanomechanical Properties to Dynamic Structure Evolution. Macromolecules 2022, 55 (11) , 4177-4199. https://doi.org/10.1021/acs.macromol.2c00076
    3. Danielle J. Mai, Charles M. Schroeder. 100th Anniversary of Macromolecular Science Viewpoint: Single-Molecule Studies of Synthetic Polymers. ACS Macro Letters 2020, 9 (9) , 1332-1341. https://doi.org/10.1021/acsmacrolett.0c00523
    4. Mehak, Gurleen Singh, Riddima Singh, Gurjaspreet Singh, Jigmat Stanzin, Harminder Singh, Gurpreet Kaur, Jandeep Singh. Clicking in harmony: exploring the bio-orthogonal overlap in click chemistry. RSC Advances 2024, 14 (11) , 7383-7413. https://doi.org/10.1039/D4RA00494A
    5. Qian Li, Lezhi Wang, Feihong Chen, Anna P. Constantinou, Theoni K. Georgiou. Thermoresponsive oligo(ethylene glycol) methyl ether methacrylate based copolymers: composition and comonomer effect. Polymer Chemistry 2022, 13 (17) , 2506-2518. https://doi.org/10.1039/D1PY01688A
    6. Graeme Moad. Trithiocarbonates in RAFT Polymerization. 2021, 359-492. https://doi.org/10.1002/9783527821358.ch9
    7. Zeqi Min, Biyi Xu, Wen Li, Afang Zhang. Combination of DNA with polymers. Polymer Chemistry 2021, 12 (13) , 1898-1917. https://doi.org/10.1039/D0PY01777A
    8. Shivani F. Patel, Charles D. Young, Charles E. Sing, Charles M. Schroeder. Nonmonotonic dependence of comb polymer relaxation on branch density in semidilute solutions of linear polymers. Physical Review Fluids 2020, 5 (12) https://doi.org/10.1103/PhysRevFluids.5.121301
    9. Fan Xiao, Zixiang Wei, Maggie Wang, Alexandra Hoff, Ying Bao, Leilei Tian. Oligonucleotide–Polymer Conjugates: From Molecular Basics to Practical Application. Topics in Current Chemistry 2020, 378 (2) https://doi.org/10.1007/s41061-020-0286-8
    10. Charles D. Young, Michael Marvin, Charles E. Sing. Conformationally averaged iterative Brownian dynamics simulations of semidilute polymer solutions. The Journal of Chemical Physics 2018, 149 (17) https://doi.org/10.1063/1.5041453
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