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Development of Single-Molecule Mechanochemical Biosensors for Ultrasensitive and Multiplex Sensing of Analytes

Mandal, Shankar
http://orcid.org/0000-0002-2653-8760
http://rave.ohiolink.edu/etdc/view?acc_num=kent1556620800317961

Abstract Details

2019, PHD, Kent State University, College of Arts and Sciences / Department of Chemistry.
A biosensor is an analytical device that utilizes recognition element to report specific binding to biological target using a physicochemical transducer element. Biosensors have a very wide range of applications including health care, point of care testing, drug discovery, environmental monitoring, biodefense, bioresearch and many others. In past few decades, biosensors have been developed with high sensitivity, specificity and usability. However, separate arrangement of target recognition and signal transduction in conventional biosensors often compromises real-time response. Moreover, to improve the sensitivity, signals are often increased from numerous molecules accumulated during various amplification processes, which introduce additional steps and increase the cost of biosensors. To address these issues, we combined analyte recognition and signal reporting via mechanochemical coupling in a single-molecule DNA template. We incorporated a DNA hairpin as a signal reporting element while recognition units are placed separately on the DNA template in a tight coupling. With an optically levitated setup in laser-tweezers instrument, DNA hairpin acts as a mechanophore, which undergoes stochastic transitions between folded and unfolded hairpin states to report biosensing events. The sensitivities were demonstrated by detecting 10 pM antibody in a Tris buffer and 100 pM in human serum in 30 minutes by incorporating a pair of antigens in the template. The sensitivities of the single-molecule mechanochemical biosensors were further increased by detecting 1 fM Hg(II) ions in environmental water samples using polyvalent recognition units in 20 minutes. The multiplexing capability of the developed biosensor was tested by detecting several miRNAs in femtomolar detection limits (LOD) in buffer and picomolar LOD in human serum in 25 minutes. We anticipated that these mechanochemical concepts and methods are instrumental for the development of novel bioanalyses and have a great contribution in the field of a new sub-discipline of chemistry: Mechanoanalytical chemistry.
Hanbin Mao, PHD (Advisor)
126 p.
Chemistry
Single-molecule technique, Optical tweezers, Biosensors, Mechanochemical sensing, Molecular tuning fork, Molecular trawl and dipstick, Ultra-sensitive, Multiplexing, Mechanoanalytical chemistry

Recommended Citations

Citations

  • Mandal, S. (2019). Development of Single-Molecule Mechanochemical Biosensors for Ultrasensitive and Multiplex Sensing of Analytes [Doctoral dissertation, Kent State University]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=kent1556620800317961

    APA Style (7th edition)

  • Mandal, Shankar. Development of Single-Molecule Mechanochemical Biosensors for Ultrasensitive and Multiplex Sensing of Analytes . 2019. Kent State University, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=kent1556620800317961.

    MLA Style (8th edition)

  • Mandal, Shankar. "Development of Single-Molecule Mechanochemical Biosensors for Ultrasensitive and Multiplex Sensing of Analytes ." Doctoral dissertation, Kent State University, 2019. http://rave.ohiolink.edu/etdc/view?acc_num=kent1556620800317961

    Chicago Manual of Style (17th edition)

kent1556620800317961
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© 2019, all rights reserved.
This open access ETD is published by Kent State University and OhioLINK.