Scaffolding carbon nanotubes into single-molecule circuitry

Goldsmith, Brett; Coroneus, John G.; Lamboy, Jorge A.; Weiss, Gregory A.; Collins, Philip G.

doi:10.1557/jmr.2008.0179

Cited by 4 publications

(4 citation statements)

References 21 publications

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“…Many researchers have investigated SWNTs coated with biomolecules or other sensitizing materials, and we have simply leveraged SWNT sensitivity by tailoring such coatings to the dilute limit of one individual molecular attachment. In fact, we have developed both covalent [63][64][65][66][67][68] and non-covalent 13,14 schemes for building single molecule devices.…”

Section: Electronic Devices For Single Molecule Recordingmentioning

confidence: 99%

Single molecule recordings of lysozyme activity

Choi

Weiss

Collins

2013

Phys. Chem. Chem. Phys.

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Single molecule bioelectronic circuits provide an opportunity to study chemical kinetics and kinetic variability with bond-by-bond resolution. To demonstrate this approach, we examined the catalytic activity of T4 lysozyme processing peptidoglycan substrates. Monitoring a single lysozyme molecule through changes in a circuit’s conductance helped elucidate unexplored and previously invisible aspects of lysozyme’s catalytic mechanism and demonstrated lysozyme to be a processive enzyme governed by 9 independent time constants. The variation of each time constant with pH or substrate crosslinking provided different insights into catalytic activity and dynamic disorder. Overall, ten lysozyme variants were synthesized and tested in single molecule circuits to dissect the transduction of chemical activity into electronic signals. Measurements show that a single amino acid with the appropriate properties is sufficient for good signal generation, proving that the single molecule circuit technique can be easily extended to other proteins.

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Section: Electronic Devices For Single Molecule Recordingmentioning

confidence: 99%

Single molecule recordings of lysozyme activity

Choi

Weiss

Collins

2013

Phys. Chem. Chem. Phys.

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“…Tailoring such coatings to the dilute limit of one individual molecular attachment has not been previously appreciated. Our past work has focused on this limit, finding that covalent (17)(18)(19)(20) and noncovalent (2)(3)(4)(5)(6) techniques each have their own advantages and disadvantages. Experimentally (21,22) and theoretically (23), covalent attachment schemes are promising and conceptually appealing.…”

Section: I-b Biofunctionalizationmentioning

confidence: 99%

Single-molecule bioelectronics

Collins

2015

Handbook of Bioelectronics

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Conceptually, extending the premise of bioelectronic interfaces down to the scale of single molecules is a straightforward goal. In practice, the challenges are purely technological. Single molecule bioelectronic devices would have to involve features much smaller than state-of-the-art semiconductor electronics, and successful design would have unique requirements for sensitivity and stability. These imposing specifications are balanced by the potential of enormous rewards, because single molecule bioelectronics would be a breakthrough technology for biochemical research and applications. By peering past the ensemble behaviors of traditional characterization, single molecule techniques aim to directly observe the stochastic fluctuations, instantaneous dynamics, and nonequilibrium behaviors that make up a molecule's full functionality. Moreover, single molecule measurements can uncover the unusual reaction trajectories of a genetically mutated protein or a receptor interacting with pharmacological inhibitors. Building a better understanding of the precise roles of proteins in complex biological processes is a grand challenge for biology, biochemistry, and biophysics in the 21 st century. These potential benefits have spurred the development of a variety of single-molecule techniques. Single molecule fluorescence, specifically Förster resonance energy transfer (FRET), has become a standard tool for single molecule biochemistry (1). Meanwhile, single molecule bioelectronics has remained elusive, despite the wide-ranging capabilities of modern solid state electronics. Recently, a very promising architecture for single molecule bioelectronics was demonstrated using carbon nanotube field effect transistors (Figure 1) (2). This next-generation, label-free nanocircuit technique successfully recorded the dynamic motions of single biomolecules, enabling the continuous recording of protein function through many thousands of binding events. The reaction kinetics of complex biochemical events were revealed in real-time with molecule-by-molecule precision to illuminate memory effects, dynamic disorder, and processive variability, all of which remain hidden in ensemble measurements (2-6). This chapter reviews the techniques of fabricating and using this new class of bioelectronic devices. The first section describes the nanotube transistors themselves, and the techniques used to generate single molecule devices. The second and third sections describe and demonstrate how the transistors can be used to monitor biomolecular activity. As examples, single molecule recordings are

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“…After fabrication, single site devices have been probed with various analytes. Exquisite sensitivity, including single molecule dynamic detection, has been demonstrated [8,9]. In addition, the presence of a point defect has been clearly shown to amplify the chemosensitivity compared to pristine SWNT devices [10].…”

Section: Single Site Molecular Sensorsmentioning

confidence: 99%

“…Critical to this testing is the use of conductive tip atomic force microscopy (AFM) techniques to map out tfhe local electronic responses of 30-60% when probed with H2 gas, but when the same measurement is performed with a Pd-decorated defect, the response is approximately one hundred fold. Experiments are fully described in [8][9][10].…”

Section: A Local Probing Of Defect Scatteringmentioning

confidence: 99%

Sensitivity of point defects in one dimensional nanocircuits

et al. 2010

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When tailored to contain a single resistive defect, one dimensional nanocircuits can realize high dynamic range, high bandwidth transduction of single molecule chemical events. The physical mechanisms behind this sensitive transduction, however, remain poorly understood. Here, we complement ongoing sensing measurements with scanning probe characterization of the electronic properties of defects. The high sensitivity of defect sites is directly probed, and is found to be in excellent agreement with a finite element model containing realistic device parameters for the defect sites. The model illuminates the most likely sensing mechanisms of these single molecule circuits, and fully supports the premise that further tailoring of the defect sites could enable the chemically selective interrogation of a wide range of complex molecular interactions.

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Scaffolding carbon nanotubes into single-molecule circuitry

Cited by 4 publications

References 21 publications

Single molecule recordings of lysozyme activity

Single molecule recordings of lysozyme activity

Single-molecule bioelectronics

Sensitivity of point defects in one dimensional nanocircuits

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