Fabrication of device with poly(N-isopropylacrylamide)-b-ssDNA copolymer brush for resistivity study

Yi Zu Liu, May Show Chen, Chih Chia Cheng, Shih Hsun Chen, Jem Kun Chen

Research output: Contribution to journalArticle

1 Citation (Scopus)

Abstract

In this study, we grafted bromo-terminated poly(N-isopropylacrylamide) (PNIPAAm) brushes onto thin gold films deposited on silicon, and then reacted with NaN3 to produce azido-terminated PNIPAAm brushes. A probe sequence of single-stranded DNA (ssDNA) with a 4-pentynoic acid succinimidyl ester unit was grafted onto the azido-terminated PNIPAAm brushes through a click reaction, resulting in the formation of block copolymer brushes. The PNIPAAm-b-ssDNA copolymer brushes formed supramolecular complexes stabilized by bio-multiple hydrogen bonds (BMHBs), which enhanced the proton transfer and thereby decreased the resistivity of the structures. In addition, the optimal operation window for DNA detection ranges from 0 to 0.2 M of NaCl concentration. Therefore, the specimens were prepared in the PBS solution at 150 mM NaCl concentration for target hybridization. The supramolecular complex state of the PNIPAAm-b-ssDNA copolymer brushes transformed into the phase-separated state after the hybridization with 0.5 ng/μL of its target DNA sequence owing to the competition between BMHBs and complementary hydrogen bonds. This phase transformation of the PNIPAAm and probe segments inhibited the proton transfer and significantly increased the resistivity at 25 °C. Moreover, there were no significant changes in the resistivity of the copolymer brushes after hybridization with the target sequence at 45 °C. These results indicated that the phase-separated state of the PNIPAAm-b-ssDNA copolymer brushes, which was generally occurred above the LCST, can be substantially generated after hybridization with its target DNA sequence. By performing the controlled experiments, in the same manner, using another sequence with lengths similar to that of the target sequence without complementarity. In addition, the sequences featuring various degrees of complementarity were exploited to verify the phase separation behavior inside the PNIPAAm-b-ssDNA copolymer thin film.

Original languageEnglish
Article number68
JournalJournal of Nanobiotechnology
Volume15
Issue number1
DOIs
Publication statusPublished - Oct 5 2017

Fingerprint

Single-Stranded DNA
Brushes
DNA
Copolymers
Fabrication
Equipment and Supplies
Hydrogen
Hydrogen bonds
Proton transfer
DNA sequences
Protons
Sodium Azide
poly-N-isopropylacrylamide
Silicon
Phase separation
Gold
Block copolymers
Esters
Phase transitions
Thin films

Keywords

  • Block copolymer brush
  • Resistivity
  • Supramolecular complex

ASJC Scopus subject areas

  • Bioengineering
  • Medicine (miscellaneous)
  • Molecular Medicine
  • Biomedical Engineering
  • Applied Microbiology and Biotechnology
  • Pharmaceutical Science

Cite this

Fabrication of device with poly(N-isopropylacrylamide)-b-ssDNA copolymer brush for resistivity study. / Liu, Yi Zu; Chen, May Show; Cheng, Chih Chia; Chen, Shih Hsun; Chen, Jem Kun.

In: Journal of Nanobiotechnology, Vol. 15, No. 1, 68, 05.10.2017.

Research output: Contribution to journalArticle

Liu, Yi Zu ; Chen, May Show ; Cheng, Chih Chia ; Chen, Shih Hsun ; Chen, Jem Kun. / Fabrication of device with poly(N-isopropylacrylamide)-b-ssDNA copolymer brush for resistivity study. In: Journal of Nanobiotechnology. 2017 ; Vol. 15, No. 1.
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AU - Chen, Jem Kun

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AB - In this study, we grafted bromo-terminated poly(N-isopropylacrylamide) (PNIPAAm) brushes onto thin gold films deposited on silicon, and then reacted with NaN3 to produce azido-terminated PNIPAAm brushes. A probe sequence of single-stranded DNA (ssDNA) with a 4-pentynoic acid succinimidyl ester unit was grafted onto the azido-terminated PNIPAAm brushes through a click reaction, resulting in the formation of block copolymer brushes. The PNIPAAm-b-ssDNA copolymer brushes formed supramolecular complexes stabilized by bio-multiple hydrogen bonds (BMHBs), which enhanced the proton transfer and thereby decreased the resistivity of the structures. In addition, the optimal operation window for DNA detection ranges from 0 to 0.2 M of NaCl concentration. Therefore, the specimens were prepared in the PBS solution at 150 mM NaCl concentration for target hybridization. The supramolecular complex state of the PNIPAAm-b-ssDNA copolymer brushes transformed into the phase-separated state after the hybridization with 0.5 ng/μL of its target DNA sequence owing to the competition between BMHBs and complementary hydrogen bonds. This phase transformation of the PNIPAAm and probe segments inhibited the proton transfer and significantly increased the resistivity at 25 °C. Moreover, there were no significant changes in the resistivity of the copolymer brushes after hybridization with the target sequence at 45 °C. These results indicated that the phase-separated state of the PNIPAAm-b-ssDNA copolymer brushes, which was generally occurred above the LCST, can be substantially generated after hybridization with its target DNA sequence. By performing the controlled experiments, in the same manner, using another sequence with lengths similar to that of the target sequence without complementarity. In addition, the sequences featuring various degrees of complementarity were exploited to verify the phase separation behavior inside the PNIPAAm-b-ssDNA copolymer thin film.

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