The nonlinear coupling between exothermic chemical reactions and a nanowire or nanotube with large axial heat conduction results in a self-propagating thermal wave guided along the nanoconduit. The resulting reaction wave induces a concomitant thermopower wave of high power density (>7 kW/kg), resulting in an electrical current along the same direction. We develop the theory of such waves and analyze them experimentally, showing that for certain values of the chemical reaction kinetics and thermal parameters, oscillating wavefront velocities are possible.
View Article and Find Full Text PDFThe ability to actively manipulate and transport single molecules in solution has the potential to revolutionize chemical synthesis and catalysis. In previous work, we developed a nanopore platform using the interior of a single-walled carbon nanotube (diameter = 1.5 nm) for the Coulter detection of single cations of Li(+), K(+), and Na(+).
View Article and Find Full Text PDFWe report the selective detection of single nitric oxide (NO) molecules using a specific DNA sequence of d(AT)(15) oligonucleotides, adsorbed to an array of near-infrared fluorescent semiconducting single-walled carbon nanotubes (AT(15)-SWNT). While SWNT suspended with eight other variant DNA sequences show fluorescence quenching or enhancement from analytes such as dopamine, NADH, L-ascorbic acid, and riboflavin, d(AT)(15) imparts SWNT with a distinct selectivity toward NO. In contrast, the electrostatically neutral polyvinyl alcohol enables no response to nitric oxide, but exhibits fluorescent enhancement to other molecules in the tested library.
View Article and Find Full Text PDFNanoparticles that possess a single covalent tether to either another particle or a surface play an increasingly important role in nanotechnology, serving as a foundation for aggregation-based plasmonic sensors, chemically assembled framework structures, and scanning probe tips. Using a theoretical approach, we explore the reaction conditions necessary to maximize singular tethering for several cases of homogeneously dispersed nanoparticles, with a particular focus on single-walled carbon nanotubes. In the limit of particles of monodisperse size and equal site reactivity, the number of tethers versus the reaction conversion is statistically described by the well-known binomial distribution, with a variance that is minimal for the single tether case.
View Article and Find Full Text PDFNaturally occurring photosynthetic systems use elaborate pathways of self-repair to limit the impact of photo-damage. Here, we demonstrate a complex consisting of two recombinant proteins, phospholipids and a carbon nanotube that mimics this process. The components self-assemble into a configuration in which an array of lipid bilayers aggregate on the surface of the carbon nanotube, creating a platform for the attachment of light-converting proteins.
View Article and Find Full Text PDFThere is significant interest in combining carbon nanotubes with semiconducting polymers for photovoltaic applications because of potential advantages from smaller exciton transport lengths and enhanced charge separation. However, to date, bulk heterojunction (BHJ) devices have demonstrated relatively poor efficiencies, and little is understood about the polymer/nanotube junction. To investigate this interface, we fabricate a planar nano-heterojunction comprising well-isolated millimeter-long single-walled carbon nanotubes underneath a poly(3-hexylthiophene) (P3HT) layer.
View Article and Find Full Text PDFUnderstanding the solution-phase dispersion of pristine, unfunctionalized graphene is important for the production of conducting inks and top-down approaches to electronics. This process can also be used as a higher-quality alternative to chemical vapor deposition. We have developed a theoretical framework that utilizes molecular dynamics simulations and the kinetic theory of colloid aggregation to elucidate the mechanism of stabilization of liquid-phase-exfoliated graphene sheets in N-methylpyrrolidone (NMP), N,N'-dimethylformamide (DMF), dimethyl sulfoxide (DMSO), γ-butyrolactone (GBL), and water.
View Article and Find Full Text PDFSeventeen different kinds of incenses were analyzed for the volatile components emitted during burning using a HS-SPME method coupled with GC-MS, in order to check their conformity to IFRA (International Fragrance Association) guidelines and 67/548/CEE Directive rules. A total of 51 volatiles were identified in the smoke of the incenses. They were represented mainly by aromatic compounds (17) and oxygenated monoterpenes (10), with esters (5) and aldehydes (4) being the most widespread volatiles in the former, and alcohols (4) and esters (4) in the latter.
View Article and Find Full Text PDFThere has been renewed interest in solar concentrators and optical antennas for improvements in photovoltaic energy harvesting and new optoelectronic devices. In this work, we dielectrophoretically assemble single-walled carbon nanotubes (SWNTs) of homogeneous composition into aligned filaments that can exchange excitation energy, concentrating it to the centre of core-shell structures with radial gradients in the optical bandgap. We find an unusually sharp, reversible decay in photoemission that occurs as such filaments are cycled from ambient temperature to only 357 K, attributed to the strongly temperature-dependent second-order Auger process.
View Article and Find Full Text PDFBiological ion channels are able to generate coherent and oscillatory signals from intrinsically noisy and stochastic components for ultrasensitive discrimination with the use of stochastic resonance, a concept not yet demonstrated in human-made analogs. We show that a single-walled carbon nanotube demonstrates oscillations in electroosmotic current through its interior at specific ranges of electric field that are the signatures of coherence resonance. Stochastic pore blocking is observed when individual cations partition into the nanotube obstructing an otherwise stable proton current.
View Article and Find Full Text PDFThere has been significant interest in using electronically contacted nanorod or nanotube arrays as gas sensors, whereby an adsorbate modifies either the impedance or the Fermi level of the array, enabling detection. Typically, such arrays demonstrate the I-V curves of a Schottky diode that is formed using a metal-semiconductor junction with rectifying characteristics. We show in this work that nanostructured Schottky diodes have a functionally different response, characteristic of the large electric field induced by the size scale of the array.
View Article and Find Full Text PDFAn emerging concept in cell signalling is the natural role of reactive oxygen species such as hydrogen peroxide (H2O2) as beneficial messengers in redox signalling pathways. The nature of H2O2 signalling is confounded, however, by difficulties in tracking it in living systems, both spatially and temporally, at low concentrations. Here, we develop an array of fluorescent single-walled carbon nanotubes that can selectively record, in real time, the discrete, stochastic quenching events that occur as H2O2 molecules are emitted from individual human epidermal carcinoma cells stimulated by epidermal growth factor.
View Article and Find Full Text PDFTheoretical calculations predict that by coupling an exothermic chemical reaction with a nanotube or nanowire possessing a high axial thermal conductivity, a self-propagating reactive wave can be driven along its length. Herein, such waves are realized using a 7-nm cyclotrimethylene trinitramine annular shell around a multiwalled carbon nanotube and are amplified by more than 10(4) times the bulk value, propagating faster than 2 m s(-1), with an effective thermal conductivity of 1.28+/-0.
View Article and Find Full Text PDFJ Diabetes Sci Technol
March 2009
This article reviews current efforts to make glucose sensors based on the inherent optical properties of single walled carbon nanotubes. The advantages of single walled carbon nanotubes over traditional organic and nanoparticle fluorophores for in vivo-sensing applications are discussed. Two recent glucose sensors made by our group are described, with the first being an enzyme-based glucose sensor that couples a reaction mediator, which quenches nanotube fluorescence, on the surface of the nanotube with the reaction of the enzyme.
View Article and Find Full Text PDFThe reactivity of graphene and its various multilayers toward electron transfer chemistries with 4-nitrobenzene diazonium tetrafluoroborate is probed by Raman spectroscopy after reaction on-chip. Single graphene sheets are found to be almost 10 times more reactive than bi- or multilayers of graphene according to the relative disorder (D) peak in the Raman spectrum examined before and after chemical reaction in water. A model whereby electron puddles that shift the Dirac point locally to values below the Fermi level is consistent with the reactivity difference.
View Article and Find Full Text PDFWhen pyrimidine-functionalized carbon nanotubes were incubated with single-stranded DNA ligase, formations of macroscopic aggregates were observed. Wet-cell transmission electron microscopy imaging revealed that the nanotubes were radially bound to form a 3D latticelike structure. These structures were not observed in control reactions lacking ligase or adenosine triphosphate.
View Article and Find Full Text PDFWe demonstrate the use of hydrogel swelling as a mechanism to reversibly induce solvatochromic shifting in single-walled carbon nanotube (SWNT) near-infrared emission within a biocompatible hydrogel. The optical sensor reports the degree of the swelled state and glucose concentration when apo-glucose oxidase is used to cross-link the hydrogel. Photoluminescence emission maxima from dispersed nanotubes in a poly(vinyl alcohol) hydrogel shift as cross-linking is increased, with a maximum of -48 meV for the (6,5) nanotube.
View Article and Find Full Text PDFControlling the morphology of membrane components at the nanometer scale is central to many next-generation technologies in water purification, gas separation, fuel cell, and nanofiltration applications. Toward this end, we report the covalent assembly of single-walled carbon nanotubes (SWNTs) into three-dimensional framework materials with intertube pores controllable by adjusting the size of organic linker molecules. The frameworks are fashioned into multilayer membranes possessing linker spacings from 1.
View Article and Find Full Text PDFA major challenge in the synthesis of nanotube or nanowire sensors is to impart selective analyte binding through means other than covalent linkages, which compromise electronic and optical properties. We synthesized a 3,4-diaminophenyl-functionalized dextran (DAP-dex) wrapping for single-walled carbon nanotubes (SWNTs) that imparts rapid and selective fluorescence detection of nitric oxide (NO), a messenger for biological signalling. The near-infrared (nIR) fluorescence of SWNT(DAP-dex) is immediately and directly bleached by NO, but not by other reactive nitrogen and oxygen species.
View Article and Find Full Text PDFIntegration of single-walled carbon nanotubes (SWNT) into complex sensing and electronic devices can necessitate the selective placement of individual nanotubes from solution onto custom-prepared surfaces. Existing studies indicate carbon nanotube adsorption can be controlled by creating hydrophilic and/or hydrophobic surfaces, depending on the nanotube surface chemistry and solvent. Various recipes exist for specific conditions, but no quantitative theoretical model describing experimental observations has been developed.
View Article and Find Full Text PDFThe 1D quantum confinement of photogenerated excitons in single-walled carbon nanotubes (SWNT) can amplify the detection of molecular adsorption to where single-molecule discrimination is realizable, even from within living cells and tissues. Toward this aim, we present a type 1 collagen film, similar to those used as 3D cell scaffolds for tissue engineering, containing embedded SWNT capable of reporting single-molecule adsorption of quenching molecules. We utilize hidden Markov modeling to link single-molecule adsorption events to rate constants for H2O2, H+, and Fe(CN)6(3-).
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