Novel nanomaterials for bioassay applications represent a rapidly progressing field of nanotechnology and nanobiotechnology. Here, we present an exploration of single-walled carbon nanotubes as a platform for investigating surface-protein and proteinprotein binding and developing highly specific electronic biomolecule detectors. Nonspecific binding on nanotubes, a phenomenon found with a wide range of proteins, is overcome by immobilization of polyethylene oxide chains. A general approach is then advanced to enable the selective recognition and binding of target proteins by conjugation of their specific receptors to polyethylene oxide-functionalized nanotubes. This scheme, combined with the sensitivity of nanotube electronic devices, enables highly specific electronic sensors for detecting clinically important biomolecules such as antibodies associated with human autoimmune diseases. R ecent years have witnessed significant interest in biological applications of novel inorganic nanomaterials such as nanocrystals (1, 2), nanowires (3), and nanotubes (4, 5) with the motivation to create new types of analytical tools for life science and biotechnology. Single-walled carbon nanotubes (SWNTs) are interesting molecular wires (diameter Ϸ1-2 nm) with unique electronic properties that have been spotlighted for future solid-state nanoelectronics (6, 7). Bridging nanotubes with biological systems, however, is a relatively unexplored area, with the exception of a few reports on nanotube probe tips for biological imaging (4), nonspecific binding (NSB) of proteins (8-10), functionalization chemistry for bioimmobilization on nanotube sidewalls (5), and one study on biocompatibility (11).Previously, we and others have shown that the electrical conductance of a nanotube is highly sensitive to its environment and varies significantly with changes in electrostatic charges and surface adsorption of various molecules (12)(13)(14). This research has hinted at possible SWNT-based miniature sensors for detecting biological molecules in fluids. Here, we systematically explore how nanotubes interact with and respond to various proteins in solution, how chemical functionalization can be used to tailor these interactions, and how the resulting understanding enables highly selective nanotube sensors for the electronic detection of proteins. Using atomic force microscopy (AFM) and quartz crystal microbalance (QCM) and electronic transport measurements, we first reveal that proteins in general exhibit a high degree of NSB on nanotubes, a phenomenon undesirable for potential biosensors. We then demonstrate a functionalization scheme involving irreversible adsorption of Tween 20 or triblock copolymer chains on nanotubes to prevent this general NSB, while at the same time enabling the binding of specific proteins of interest that can be detected electronically without the need for labeling. Further, we demonstrate specific detection of mAbs to the human autoantigen U1A, a prototype target of the autoimmune response in patients with systemic lupu...
The ability to form integrated circuits on flexible sheets of plastic enables attributes (for example conformal and flexible formats and lightweight and shock resistant construction) in electronic devices that are difficult or impossible to achieve with technologies that use semiconductor wafers or glass plates as substrates. Organic small-molecule and polymer-based materials represent the most widely explored types of semiconductors for such flexible circuitry. Although these materials and those that use films or nanostructures of inorganics have promise for certain applications, existing demonstrations of them in circuits on plastic indicate modest performance characteristics that might restrict the application possibilities. Here we report implementations of a comparatively high-performance carbon-based semiconductor consisting of sub-monolayer, random networks of single-walled carbon nanotubes to yield small- to medium-scale integrated digital circuits, composed of up to nearly 100 transistors on plastic substrates. Transistors in these integrated circuits have excellent properties: mobilities as high as 80 cm(2) V(-1) s(-1), subthreshold slopes as low as 140 m V dec(-1), operating voltages less than 5 V together with deterministic control over the threshold voltages, on/off ratios as high as 10(5), switching speeds in the kilohertz range even for coarse (approximately 100-microm) device geometries, and good mechanical flexibility-all with levels of uniformity and reproducibility that enable high-yield fabrication of integrated circuits. Theoretical calculations, in contexts ranging from heterogeneous percolative transport through the networks to compact models for the transistors to circuit level simulations, provide quantitative and predictive understanding of these systems. Taken together, these results suggest that sub-monolayer films of single-walled carbon nanotubes are attractive materials for flexible integrated circuits, with many potential areas of application in consumer and other areas of electronics.
Single-walled carbon nanotubes (SWNTs) have many exceptional electronic properties. Realizing the full potential of SWNTs in realistic electronic systems requires a scalable approach to device and circuit integration. We report the use of dense, perfectly aligned arrays of long, perfectly linear SWNTs as an effective thin-film semiconductor suitable for integration into transistors and other classes of electronic devices. The large number of SWNTs enable excellent device-level performance characteristics and good device-to-device uniformity, even with SWNTs that are electronically heterogeneous. Measurements on p- and n-channel transistors that involve as many as approximately 2,100 SWNTs reveal device-level mobilities and scaled transconductances approaching approximately 1,000 cm(2) V(-1) s(-1) and approximately 3,000 S m(-1), respectively, and with current outputs of up to approximately 1 A in devices that use interdigitated electrodes. PMOS and CMOS logic gates and mechanically flexible transistors on plastic provide examples of devices that can be formed with this approach. Collectively, these results may represent a route to large-scale integrated nanotube electronics.
The enormous amount of basic research into carbon nanotubes has sparked interest in the potential applications of these novel materials. One promising use of carbon nanotubes is as fillers in a composite material to improve mechanical behaviour, electrical transport and thermal transport. For composite materials with high thermal conductivity, the thermal conductance across the nanotube-matrix interface is of particular interest. Here we use picosecond transient absorption to measure the interface thermal conductance (G) of carbon nanotubes suspended in surfactant micelles in water. Classical molecular dynamics simulations of heat transfer from a carbon nanotube to a model hydrocarbon liquid are in agreement with experiment. Our findings indicate that heat transport in a nanotube composite material will be limited by the exceptionally small interface thermal conductance (G approximately 12 MW m(-2) K(-1)) and that the thermal conductivity of the composite will be much lower than the value estimated from the intrinsic thermal conductivity of the nanotubes and their volume fraction.
The interface between biological molecules and novel nanomaterials is important to developing new types of miniature devices for biological applications. Here, the streptavidin/biotin system is used to investigate the adsorption behavior of proteins on the sides of single-walled carbon nanotubes (SWNTs). Functionalization of SWNTs by coadsorption of a surfactant and poly(ethylene glycol) is found to be effective in resisting nonspecific adsorption of streptavidin. Specific binding of streptavidin onto SWNTs is achieved by co-functionalization of nanotubes with biotin and protein-resistant polymers.
Nanotube/nanoparticle hybrid structures are prepared by forming Au and Pt nanoparticles on the sidewalls of single-walled carbon nanotubes. Reducing agent or catalyst-free electroless deposition, which purely utilizes the redox potential difference between Au3+, Pt2+, and the carbon nanotube, is the main driving force for this reaction. It is also shown that carbon nanotubes act as a template for wire-like metal structures. The successful formation of the hybrid structures is monitored by atomic force microscopy (AFM) and electrical measurements.
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