Abstract

The study of biomolecular interactions at the single-molecule level holds great potential for both basic science and biotechnology applications. Single-molecule studies often rely on fluorescence-based reporting, with signal levels limited by photon emission from single optical reporters. The point-functionalized carbon nanotube transistor, known as the single-molecule field-effect transistor, is a bioelectronics alternative based on intrinsic molecular charge that offers significantly higher signal levels for detection. Such devices are effective for characterizing DNA hybridization kinetics and thermodynamics and enabling emerging applications in genomic identification. In this work, we show that hybridization kinetics can be directly controlled by electrostatic bias applied between the device and the surrounding electrolyte. We perform the first single-molecule experiments demonstrating the use of electrostatics to control molecular binding. Using bias as a proxy for temperature, we demonstrate the feasibility of detecting various concentrations of 20-nt target sequences from the Ebolavirus nucleoprotein gene in a constant-temperature environment.

Highlights

  • The study of biomolecular interactions at the single-molecule level holds great potential for both basic science and biotechnology applications

  • Post fabrication, unfunctionalized single-walled carbon nanotube (SWCNT) devices are subsequently passivated with a 30-nm-thick e-beam-exposed polymethyl methacrylate (PMMA)-resist layer, leaving a 30-nm deep exposed ‘window’ used to confine the covalent modification

  • We have developed an all-electronic approach for measuring the kinetics and thermodynamics of DNA hybridization and melting as a function of temperature and electrostatic bias applied through the surrounding electrolyte

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Summary

Introduction

The study of biomolecular interactions at the single-molecule level holds great potential for both basic science and biotechnology applications. The point-functionalized carbon nanotube transistor, known as the single-molecule field-effect transistor, is a bioelectronics alternative based on intrinsic molecular charge that offers significantly higher signal levels for detection. Such devices are effective for characterizing DNA hybridization kinetics and thermodynamics and enabling emerging applications in genomic identification. Point-functionalized single-walled carbon nanotube (SWCNT) devices[15] have emerged as an all-electronic, label-free, singlemolecule detection platform This single-molecule field-effect transistor (smFET) is characterized by a conductance that is sensitive to charges localized within a few Debye lengths of a point defect that is generated on the SWCNT sidewall[16]. Hybridization and melting kinetics become more complex with longer probes because of the formation of relatively stable intermediates

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