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A series of vancomycin-modified nanoparticles were developed and employed in magnetic confinement assays to isolate a variety of Gram-positive and Gram-negative bacteria from aqueous solution. We determined that the orientation/architecture of vancomycin on the surface of the nanoparticles and the overall surface coverage is critical in mediating fast and effective interactions between the nanoparticle and the pathogen cell wall surface and only one orientation/architecture in a series of modified nanoparticles leads to the efficient and reproducible capture of several important pathogenic bacteria. Interestingly, as the nanoparticles increase in diameter (from approximately 50 to 2800 nm), it is necessary to incorporate a long linker between the nanoparticle surface and the vancomycin moiety in order for the surface bound probe to efficiently confine Gram-positive bacteria. Finally, we also determined that the time required for efficient labeling and subsequent magnetic confinement significantly decreases as the size of the nanoparticle and the vancomycin surface coverage on the nanoparticle increases. As disease detection technologies transition to "lab-on-a-chip" based platforms it is necessary to develop strategies to effectively and inexpensively preconcentrate cells from large volume to volumes more amenable to these types of microfluidic devices. These small molecule-modified superparamagnetic nanoparticles can provide a means by which this can be accomplished.
ACS Nano 2008 Sep 23
PMID:Vancomycin-modified nanoparticles for efficient targeting and preconcentration of Gram-positive and Gram-negative bacteria. 1920 16

Complementary symmetry (CS) Boolean logic utilizes both p- and n-type field-effect transistors (FETs) so that an input logic voltage signal will turn one or more p- or n-type FETs on, while turning an equal number of n- or p-type FETs off. The voltage powering the circuit is prevented from having a direct pathway to ground, making the circuit energy efficient. CS circuits are thus attractive for nanowire logic, although they are challenging to implement. CS logic requires a relatively large number of FETs per logic gate, the output logic levels must be fully restored to the input logic voltage level, and the logic gates must exhibit high gain and robust noise margins. We report on CS logic circuits constructed from arrays of 16 nm wide silicon nanowires. Gates up to a complexity of an XOR gate (6 p-FETs and 6 n-FETs) containing multiple nanowires per transistor exhibit signal restoration and can drive other logic gates, implying that large scale logic can be implemented using nanowires. In silico modeling of CS inverters, using experimentally derived look-up tables of individual FET properties, is utilized to provide feedback for optimizing the device fabrication process. Based upon this feedback, CS inverters with a gain approaching 50 and robust noise margins are demonstrated. Single nanowire-based logic gates are also demonstrated, but are found to exhibit significant device-to-device fluctuations.
ACS Nano 2008 Sep 23
PMID:Complementary symmetry nanowire logic circuits: experimental demonstrations and in silico optimizations. 1920 17

Janus nanoparticles have been synthesized consisting of approximately 5 nm magnetite nanoparticles coated on one side with a pH-dependent and temperature-independent polymer (poly(acrylic acid), PAA), and functionalized on the other side by a second (tail) polymer that is either a pH-independent polymer (polystyrene sodium sulfonate, PSSNa) or a temperature-dependent polymer (poly(N-isopropyl acrylamide), PNIPAM). These Janus nanoparticles are dispersed stably as individual particles at high pH values and low temperatures, but can self-assemble at low pH values (PSSNa) or at high temperatures (>31 degrees C) (PNIPAM) to form stable dispersions of clusters of approximately 80-100 nm in hydrodynamic diameter. The Janus nanoparticle compositions were verified using FTIR and XPS, and their structures observed directly by TEM. Their clustering behavior is analyzed by dynamic light scattering and zeta potential measurements.
ACS Nano 2008 Sep 23
PMID:Reversible clustering of pH- and temperature-responsive Janus magnetic nanoparticles. 1920 18

We present a novel approach to construct hollow polymeric microcontainers that can be remotely addressed using a low-power near-infrared laser to release encapsulated materials. Microshells possessing walls with aggregates of gold nanoparticles are found to release encapsulated materials upon near-IR irradiation, while shells containing the same amount of nonaggregated gold nanoparticles did not release their contents. The permeability of thermally shrunk microcapsules to dextran molecules is the lowest for shells containing nonaggregated nanoparticles and the highest for microcapsules with no nanoparticles. The wall thickness, roughness, influence of concentration of encapsulated materials, and general shrinking behavior of the microcapsules are studied. Aggregation of nanoparticles increases the absorption coefficient in the near-infrared part of electromagnetic spectrum. The temperature increase upon near-infrared laser illumination for different gold nanoparticle distributions is simulated. Important implications of this approach are expected in development of drug delivery systems as well as in temperature- and light-sensitive materials and membranes.
ACS Nano 2008 Sep 23
PMID:Toward self-assembly of nanoparticles on polymeric microshells: near-IR release and permeability. 1920 19

An atomic force microscope and the colloidal probe technique are used to probe the interaction between a hydrophobic particle and a hydrophobic surface in water. The characteristics of the observed force curves strongly suggest that a gas bubble is formed when the particle is moved toward the surface and that the bubble ruptures when the particle subsequently is retracted from the surface. We demonstrate that this type of interaction is not unique for hydrophobic surfaces in water since the interaction between hydrophilic surfaces in air provides very similar force curves. However, the interaction between hydrophobic surfaces vanish if water is replaced by an organic solvent with low polarity. The bridging bubble model is employed to explain the hysteresis observed between approach and retraction force traces and experimental conditions where the hysteresis can be almost eliminated are identified. Finally, it is demonstrated that the hydrophobic interaction is strongly temperature dependent and this dependence can be attributed mainly to the decreasing solubility of air in water with increasing temperature.
ACS Nano 2008 Sep 23
PMID:Force trace hysteresis and temperature dependence of bridging nanobubble induced forces between hydrophobic surfaces. 1920 20

We report the novel fabrication of a highly sensitive, selective, fast responding, and affordable amperometric glucose biosensor using exfoliated graphite nanoplatelets (xGnPs) decorated with Pt and Pd nanoparticles. Nafion was used to solubilize metal-decorated graphite nanoplatelets, and a simple cast method with high content organic solvent (85 wt %) was used to prepare the biosensors. The addition of precious metal nanoparticles such as platinum (Pt) and palladium (Pd) to xGnP increased the electroactive area of the electrode and substantially decreased the overpotential in the detection of hydrogen peroxide. The Pt-xGnP glucose biosensor had a sensitivity of 61.5+/-0.6 microA/(mM x cm(2)) and gave a linear response up to 20 mM. The response time and detection limit (S/N=3) were determined to be 2 s and 1 microM, respectively. Therefore, this novel glucose biosensor based on the Pt nanoparticle coated xGnP is among the best reported to date in both sensing performance and production cost. In addition, the effects of metal nanoparticle loading and the particle size on the biosensor performance were systematically investigated.
ACS Nano 2008 Sep 23
PMID:Nanometal-decorated exfoliated graphite nanoplatelet based glucose biosensors with high sensitivity and fast response. 1920 21

Surface modification of carbon nanotubes (CNTs) has been widely studied for some years. However, the asymmetric modification of individual CNTs with different molecular species/nanoparticles at the two end-tips or along the nanotube length is only a recent development. As far as we are aware, no attempt has so far been made to asymmetrically functionalize individual CNTs with moieties of opposite charges. In this paper, we have demonstrated a simple, but effective, asymmetric modification of the sidewall of CNTs with oppositely charged moieties by plasma treatment and pi-pi stacking interaction. The as-prepared asymmetrically sidewall-functionalized CNTs can be used as a platform for bottom-up self-assembly of complex structures or can be charge-selectively self-assembled onto and/or between electrodes with specific biases under an appropriate applied voltage for potential device applications.
ACS Nano 2008 Sep 23
PMID:Asymmetrically charged carbon nanotubes by controlled functionalization. 1920 22

Introducing small amounts of additives into polymerization reactions to produce conducting polymers can have a profound impact on the resulting polymer morphology. When an oligomer such as aniline dimer is added to the polymerization of aniline, the nanofibers produced are longer and less entangled than those typically observed. The addition of aniline dimer can even induce nanofiber formation under synthetic conditions that generally do not favor a nanofibrillar morphology. This finding can be extended to both the synthesis of polythiophene and polypyrrole nanofibers. The traditional oxidative polymerization of thiophene or pyrrole only produces agglomerated particles. However, when minute amounts of thiophene or pyrrole oligomers are added to the reaction, the resulting polymers possess a nanofibrillar morphology. These results reveal important insights into a semirigid rod nucleation phenomenon that has hitherto been little explored. When polyaniline nucleates homogeneously, surface energy requirements necessitate the formation of ordered nuclei which leads to the directional polymerization of aniline. This ultimately leads to the one-dimensional nanofibrillar morphology observed in the final product. The synthetic procedures developed here are simple, scalable, and do not require any templates or other additives that are not inherent to the polymer.
ACS Nano 2008 Sep 23
PMID:Toward an understanding of the formation of conducting polymer nanofibers. 1920 23

The control of the structure of oxide-supported metal nanoparticles is crucial in determining their properties and possible applications. Here, building principles are derived for predicting the epitaxies of metal nanoparticles on square-symmetry oxide surfaces. Unusual phases are found for an appropriate choice of the metal-oxide pair, where nanoparticles with hcp structure are stabilized for fcc metals such as Ni, Pd, and Pt, or for Co in a size range in which Co has typically nonhcp arrangements. These predictions are supported by a comparison with available experimental data on Ni/MgO(100) nanodots, and generalized to a whole class of metal-oxide systems of great potential interest, such as Pd and Pt on CaO, Ni on CoO, and Co on MgO. The atomistic features of the nanoparticles in turn suggest that these materials should possess peculiar properties; in particular, the facets exposed by the nanodots reveal adsorption sites with unusual geometry of possible effect on their catalytic properties, while the destabilization of stacking faults and the structural deformations observed for these particles are expected to influence their magnetic behavior.
ACS Nano 2008 Sep 23
PMID:Interface-stabilized phases of metal-on-oxide nanodots. 1920 24

We demonstrate the synthesis of a series of spin-labeled curved oligomers to determine their end-to-end lengths and distance distributions using electron spin resonance. We synthesize shape-persistent macromolecules from conformationally restricted, asymmetric monomers that are coupled through pairs of amide bonds to create water-soluble, spiro-ladder oligomers with well-defined three-dimensional structures. We synthesized seven different macromolecules, each containing eight monomers but differing in the sequence to create macromolecules with different curved shapes. The ends of the oligomers were labeled with nitroxide spin probes, and double electron-electron resonance (DEER) electron spin resonance (ESR) experiments were carried out to obtain quantitative information about the shapes and flexibility of the oligomers. The most probable end-to-end distance of the oligomers ranges from 23 to 36 A, a range of length that we previously accessed by assembling rod-like homo-oligomers that contain 4-8 bisamino acid monomers. The relative distances measured for the oligomers confirm that, by varying the sequence of an oligomer, we are able to control its shape. The shapes of the ESR-derived population distributions allow us to compare the degree of shape persistence and flexibility of spiro-ladder oligomers to other well-studied nanoscale molecular structures such as p-phenylethynylenes.
ACS Nano 2008 Sep 23
PMID:Distance distributions of end-labeled curved bispeptide oligomers by electron spin resonance. 1920 25


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