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At least 487 records · Page 27Linked to original sources
PubMed2004

Effect of macromolecular crowding on DNA:Au nanoparticle bioconjugate assembly.

DNA:Au nanosphere bioconjugates have applications in biosensing and in the bottom-up assembly of materials. These bioconjugates can be selectively assembled into three-dimensional aggregates upon addition of complementary DNA oligonucleotides and can be dissociated by heating above a melting transition temperature at which the DNA duplexes are denatured. Herein we describe the impact of polymeric solutes on the thermal denaturation behavior of DNA:Au nanoparticle bioconjugate assemblies. Polymeric solutes can dramatically impact biochemical reactions via macromolecular crowding. Poly(ethylene glycol)s (PEGs) and dextrans of varying molecular weights were used as crowding reagents. While both PEG and dextran increased the stability of DNA:Au aggregates, melting transition temperatures in the presence of PEG were impacted more significantly. Polymer molecular weight was less important than polymer chemistry and weight percent in solution. For a high (15%) weight percent of PEG, aggregation was observed even in the absence of complementary oligonucleotides. These results underscore the importance of polymer chemistry in addition to physical volume exclusion in macromolecular crowding and point to the importance of understanding these effects when designing biorecognition-based nanoparticle assembly schemes in complex matrixes (i.e., any involving polymeric solutes).

Base Sequence↗
PubMed2004

Photopolymerization of poly(ethylene glycol) diacrylate on eosin-functionalized surfaces.

We describe a new method that allows photopolymerization of hydrogels to occur on surfaces functionalized with eosin. In this work, glass and silicon surfaces were derivatized with eosin and photopolymerization was carried out using visible light (514 nm). This mild condition may have advantages over methods that use ultraviolet (UV) light (e.g., for encapsulation of cells and proteins, in drug screening, or in biosensing applications). The hydrogel formed on the modified surface is remarkably stable for an extended period of time. The resultant hydrogel was hydrated for more than 18 months without suffering delamination from the substrate surface. This strongly suggests covalent attachment of the hydrogel to the surface. Contact angle titration measurements and X-ray photoelectron spectroscopy analysis of eosin surfaces before and after irradiation in the presence of triethanolamine suggest that the eosin radical is responsible for the covalent attachment of the gel onto the substrate surface. This method allows for 2-D patterning of hydrogels, which is demonstrated here using the microcontact printing technique. However, noncontact photolithography could be used to form similar patterns by directing light through a mask. This method can be easily implemented to form arrays of fluorophores and proteins in situ.

Eosine Yellowish-(YS)↗
PubMed2005

Self-assembled monolayers of peptide nucleic acids on gold surfaces: a spectroscopic study.

We have characterized self-assembled monolayers (SAMs) of thiol-derivatized peptide nucleic acid (PNA) chains adsorbed on gold surfaces by using reflection absorption infrared spectroscopy (RAIRS) and X-ray photoemission spectroscopy (XPS) techniques. We have found that the molecular orientation of PNAs strongly depends on surface coverage. At low coverage, PNA chains lie flat on the surface, while at high coverage, PNA molecules realign their molecular axes with the surface normal and form SAMs without the need of co-immobilization of spacers or other adjuvant molecules. The change in the molecular orientation has been studied by infrared spectroscopy and it has been confirmed by atomic force microscopy (AFM). PNA immobilization has been followed by analyzing the N(1s) XPS core-level peak. We show that the fine line shape of the N(1s) core-level peak at optimal concentration for biosensing is due to a chemical shift. A combination of the above-mentioned techniques allow us to affirm that the structure of the SAMs is stabilized by molecule-molecule interactions through noncomplementary adjacent nucleic bases.

Chromatography, High Pressure Liquid↗
PubMed2006

Composition-tunable properties of amphiphilic comb copolymers containing protected methacrylic acid groups for multicomponent protein patterning.

Methods to micropattern multiple protein components on surfaces under mild conditions are of interest for biosensing, proteomics, and fundamental studies in cell biology. Here, we report on the composition-dependent thin-film solubility behavior of o-nitrobenzyl methacrylate (oNBMA, a protected form of methacrylic acid)/methyl methacrylate (MMA)/poly(ethylene glycol) methacrylate (PEGMA) random terpolymers, materials which are promising as aqueous-processible photoresists. Over a broad range of terpolymer compositions, these materials formed initially water-insoluble films, which, upon UV irradiation, rapidly dissolved in aqueous solutions above a critical pH. This threshold pH ranged from approximately 5-7 depending upon the copolymer composition and decreased as the relative ratio of MMA to PEGMA in the copolymers decreased. In addition, in a narrow window of compositions near 35:0:65 oNBMA/MMA/PEGMA (wt ratio), an inverse behavior was observed: thin films that were initially water soluble became kinetically stable in aqueous solutions after UV exposure. The time for these films to completely dissolve was hours rather than seconds, and the rate of dissolution was both temperature- and pH-dependent. This behavior is consistent with a transient stability imparted by inter- and intramolecular hydrogen bonding in the film. Using copolymers of this composition as negative tone photoresists, we demonstrated patterning of two proteins into two discrete regions of a surface. The selective solubility of the resist copolymer allows the entire patterning process to be completed using only biological buffers as solvents and across a temperature range between 4 and 37 degrees C without subjecting either protein to ultraviolet irradiation or dehydration. These materials are thus of interest for complex surface photopatterning under mild aqueous conditions.

Journal Article↗
PubMed2006

Porous thin films based on photo-cross-linked star-shaped poly(D,L-lactide)s.

Self-assembly processes and subsequent photo-cross-linking were used to generate cross-linked, ordered microporous structures on the surfaces of well defined four-arm star-shaped poly(D,L-lactide) (PDLLA) thin films. The four-arm star-shaped PDLLAs were synthesized using an ethoxylated pentaerythritol initiator. Solutions of the PDLLAs were cast in a humid environment, and upon solvent evaporation, ordered honeycomb structures (or breath figures) were obtained. Correlations between molar mass, polymer solution viscosity, and pore dimensions were established. The average pore dimension decreased with increasing polymer solution concentration, and a linear relationship was observed between relative humidity and average pore dimensions. Highly ordered microporous structures were also developed on four-arm star-shaped methacrylate-modified PDLLA (PDLLA-UM) thin films. Subsequent photo-cross-linking resulted in more stable PDLLA porous films. The photo-cross-linked films were insoluble, and the honeycomb structures were retained despite solvent exposure. Free-standing, structured PDLLA-UM thin films were obtained upon drying for 24 h. Ordered microporous films based on biocompatible and biodegradable polymers, such as PDLLA, offer potential applications in biosensing and biomedical applications.

Cross-Linking Reagents↗
PubMed2007

Reversible vesicle restraint in response to spatiotemporally controlled electrical signals: a bridge between electrical and chemical signaling modes.

Microelectronic devices employ electrons for signaling whereas the nervous system signals using ions and chemicals. Bridging these signaling differences would benefit applications that range from biosensing to neuroprosthetics. Here, we report the use of localized electrical signals to perform an operation common to chemical signaling in the nervous system. Specifically, we employ electrical signals to restrain vesicles reversibly. We perform this operation using the stimuli-responsive aminopolysaccharide chitosan that is able to electrodeposit onto cathode surfaces in response to localized electrical stimuli. We show that surfactant-vesicles and liposomes can be co-deposited with chitosan and are entrapped (i.e., restrained) within the deposited film's matrix. Vesicle co-deposition could be controlled spatially and temporally using microfabricated wafers with independent electrode addresses. Finally, we show that vesicles restrained within the deposited chitosan matrix can be mobilized under mildly acidic conditions (pH <6.5) that resolubilize chitosan. Potentially, the ability to restrain and mobilize chemical signals that are segregated within vesicles may allow microfluidic systems to access the rich diversity offered by chemical signaling.

Animals↗
PubMedDate not supplied

Capillary electrophoresis of poly(amidoamine) dendrimers: from simple derivatives to complex multifunctional medical nanodevices.

Multifunctional poly(amidoamine) (PAMAM) dendrimer-based nanodevices provide novel nanoplatforms for targeting, imaging, and treatment of cancers in vitro and in vivo. Generational, skeletal, and substitutional dispersities are always present in dendrimer-based medical nanodevices. Molecular distribution plays a central role for one to evaluate the quality of PAMAM materials for medical applications. Capillary electrophoresis (CE) has been extensively used as a characterization technique to analyze a range of PAMAM dendrimers, from simple PAMAM derivatives to complex multifunctional PAMAM nanodevices. This review reports the recent advances in the analysis and characterization of a variety of PAMAM dendrimer-based nanoparticles ranging from polycationic and polyanionic PAMAM derivatives to PAMAMs of different generations and defined substitutions, and to complex multifunctional PAMAM nanodevices containing targeting ligands, dyes, and drugs. Understanding the structural complexity of dendrimer nanodevices is crucial for their use as multifunctional imaging, targeting, and cancer therapeutic devices, as well as for their use in biosensing, diagnostics, and control of biological systems.

Amides↗
PubMed2005

Multiplexed hybridization detection with multicolor colocalization of quantum dot nanoprobes.

We demonstrate a hybridization detection method using multicolor oligonucleotide-functionalized quantum dots as nanoprobes. In the presence of various target sequences, combinatorial self-assembly of the nanoprobes via independent hybridization reactions leads to the generation of discernible sequence-specific spectral codings. Detection of single-molecule hybridization is achieved by measuring colocalization of individual nanoprobes. Genetic analysis for anthrax pathogenicity through simultaneous detection of multiple relevant sequences is demonstrated using this novel biosensing method as proof-of-concept.

Bacillus anthracis↗
PubMed2006

Piezoelectric and semiconducting coupled power generating process of a single ZnO belt/wire. A technology for harvesting electricity from the environment.

This paper presents the experimental observation of piezoelectric generation from a single ZnO wire/belt for illustrating a fundamental process of converting mechanical energy into electricity at nanoscale. By deflecting a wire/belt using a conductive atomic force microscope tip in contact mode, the energy is first created by the deflection force and stored by piezoelectric potential, and later converts into piezoelectric energy. The mechanism of the generator is a result of coupled semiconducting and piezoelectric properties of ZnO. A piezoelectric effect is required to create electric potential of ionic charges from elastic deformation; semiconducting property is necessary to separate and maintain the charges and then release the potential via the rectifying behavior of the Schottky barrier at the metal-ZnO interface, which serves as a switch in the entire process. The good conductivity of ZnO is rather unique because it makes the current flow possible. This paper demonstrates a principle for harvesting energy from the environment. The technology has the potential of converting mechanical movement energy (such as body movement, muscle stretching, blood pressure), vibration energy (such as acoustic/ultrasonic wave), and hydraulic energy (such as flow of body fluid, blood flow, contraction of blood vessels) into electric energy that may be sufficient for self-powering nanodevices and nanosystems in applications such as in situ, real-time, and implantable biosensing, biomedical monitoring, and biodetection.

Electric Conductivity↗
PubMed2002

Vitellogenin induction in Cyprinus carpio treated with 17beta-estradiol and 4-nonylphenol.

The aim of the present study was to demonstrate induction of vitellogenin in the common carp (Cyprinus carpio) as a biomarker for monitoring freshwater ecosystems. Sexually undifferentiated specimens of common carp were treated experimentally with 17beta-estradiol and increasing doses of 4-nonylphenol and levels of plasma Vtg were measured in order to: 1) validate an ELISA assay for plasma Vtg in the common carp using the polyclonal rabbit anti-salmon Vtg antibody AA1 (Biosense, Norway); 2) check the sensitivity of carp juveniles in producing Vtg in response to estrogen stimulation. The group treated with 17beta-estradiol showed high induction (156%) with respect to controls, also groups treated with 4-nonylphenol showed induction of Vtg. The group treated with 100 mg kg(-1) b.wt showed an induction of 61%. A statistically significant correlation was found between dose and response. This preliminary study demonstrate a response to the ELISA assay for Vtg in the common carp using rabbit anti-salmon antibody AA1. With further evidence the tested biomarker might be proposed for large scale monitoring of estrogenic effects caused by pollution in urban and industrial effluents.

Animals↗
PubMed2003

Real-time cardiac catheter navigation on three-dimensional CT images.

INTRODUCTION: Targets for ablation of atrial fibrillation, atrial flutter, and non-idiopathic ventricular tachycardia are increasingly being selected based on anatomic considerations. Because fluoroscopy provides only limited information about the relationship between catheter positions and cardiac structures, and is associated with radiation risk, other approaches to mapping may be beneficial. METHODS: The spatial and temporal information of an electromagnetic catheter tip position sensing system (Magellan, Biosense Inc.) was superimposed on a three-dimensional (3D) CT of the chest in swine using fiducial markers for image registration. Position and orientation of a 6 French catheter with an electromagnetic sensor was displayed in real-time on a corresponding 3D-CT. Catheter navigation within the heart and the great vessels was guided by detailed knowledge about catheter location in relation to cardiac anatomy. RESULTS: Anatomic structures including the atrial septum, pulmonary veins, and valvular apparatus were easily identified and used to direct catheter navigation. During the right heart examination, the catheter was navigated through the superior and inferior vena cava to predetermined anatomic locations in right atrium, right ventricle and pulmonary artery. The ablation catheter was also navigated successfully from the aorta through the aortic valve in the left ventricle. No complication was encountered during the experiments. The accuracy and precision of this novel approach to mapping was 4.69 +/- 1.70 mm and 2.22 +/- 0.69 mm, respectively. CONCLUSIONS: Real-time display of catheter position and orientation on 3D-CT scans allows accurate and precise catheter navigation in the heart. The detailed anatomic information may improve anatomically based procedures like pulmonary vein ablation and has the potential to decrease radiation times.

Animals↗
PubMed2003

Ultra-high-Q toroid microcavity on a chip.

The circulation of light within dielectric volumes enables storage of optical power near specific resonant frequencies and is important in a wide range of fields including cavity quantum electrodynamics, photonics, biosensing and nonlinear optics. Optical trajectories occur near the interface of the volume with its surroundings, making their performance strongly dependent upon interface quality. With a nearly atomic-scale surface finish, surface-tension-induced microcavities such as liquid droplets or spheres are superior to all other dielectric microresonant structures when comparing photon lifetime or, equivalently, cavity Q factor. Despite these advantageous properties, the physical characteristics of such systems are not easily controlled during fabrication. It is known that wafer-based processing of resonators can achieve parallel processing and control, as well as integration with other functions. However, such resonators-on-a-chip suffer from Q factors that are many orders of magnitude lower than for surface-tension-induced microcavities, making them unsuitable for ultra-high-Q experiments. Here we demonstrate a process for producing silica toroid-shaped microresonators-on-a-chip with Q factors in excess of 100 million using a combination of lithography, dry etching and a selective reflow process. Such a high Q value was previously attainable only by droplets or microspheres and represents an improvement of nearly four orders of magnitude over previous chip-based resonators.

Journal Article↗
PubMed2003

Controlling anisotropic nanoparticle growth through plasmon excitation.

Inorganic nanoparticles exhibit size-dependent properties that are of interest for applications ranging from biosensing and catalysis to optics and data storage. They are readily available in a wide variety of discrete compositions and sizes. Shape-selective synthesis strategies now also yield shapes other than nanospheres, such as anisotropic metal nanostructures with interesting optical properties. Here we demonstrate that the previously described photoinduced method for converting silver nanospheres into triangular silver nanocrystals--so-called nanoprisms--can be extended to synthesize relatively monodisperse nanoprisms with desired edge lengths in the 30-120 nm range. The particle growth process is controlled using dual-beam illumination of the nanoparticles, and appears to be driven by surface plasmon excitations. We find that, depending on the illumination wavelengths chosen, the plasmon excitations lead either to fusion of nanoprisms in an edge-selective manner or to the growth of the nanoprisms until they reach their light-controlled final size.

Journal Article↗
PubMed2005

A synthetic multicellular system for programmed pattern formation.

Pattern formation is a hallmark of coordinated cell behaviour in both single and multicellular organisms. It typically involves cell-cell communication and intracellular signal processing. Here we show a synthetic multicellular system in which genetically engineered 'receiver' cells are programmed to form ring-like patterns of differentiation based on chemical gradients of an acyl-homoserine lactone (AHL) signal that is synthesized by 'sender' cells. In receiver cells, 'band-detect' gene networks respond to user-defined ranges of AHL concentrations. By fusing different fluorescent proteins as outputs of network variants, an initially undifferentiated 'lawn' of receivers is engineered to form a bullseye pattern around a sender colony. Other patterns, such as ellipses and clovers, are achieved by placing senders in different configurations. Experimental and theoretical analyses reveal which kinetic parameters most significantly affect ring development over time. Construction and study of such synthetic multicellular systems can improve our quantitative understanding of naturally occurring developmental processes and may foster applications in tissue engineering, biomaterial fabrication and biosensing.

4-Butyrolactone↗
PubMed2005

Chemically tailorable colloidal particles from infinite coordination polymers.

Micrometre- and nanometre-sized particles play important roles in many applications, including catalysis, optics, biosensing and data storage. Organic particles are usually prepared through polymerization of suitable monomers or precipitation methods. In the case of inorganic materials, particle fabrication tends to involve the reduction of a metal salt, or the controlled mixing of salt solutions supplying a metal cation and an elemental anion (for example, S2-, Se2-, O2-), respectively; in some instances, these methods even afford direct control over the shape of the particles produced. Another class of materials are metal-organic coordination polymers, which are based on metal ions coordinated by polydentate organic ligands and explored for potential use in catalysis, gas storage, nonlinear optics and molecular recognition and separations. In a subset of these materials, the use of organometallic complexes as ligands (so-called metalloligands) provides an additional level of tailorability, but these materials have so far not yet been fashioned into nano- or microparticles. Here we show that simple addition of an initiation solvent to a precursor solution of metal ions and metalloligands results in the spontaneous and fully reversible formation of a new class of metal-metalloligand particles. We observe initial formation of particles with diameters of a few hundred nanometres, which then coalesce and anneal into uniform and smooth microparticles. The ease with which these particles can be fabricated, and the ability to tailor their chemical and physical properties through the choice of metal and organic ligand used, should facilitate investigations of their scope for practical applications.

Journal Article↗
PubMed2004

Oxidation-responsive polymeric vesicles.

Vesicles formed in water by synthetic macro-amphiphiles have attracted much attention as nanocontainers having properties that extend the physical and chemical limits of liposomes. We sought to develop ABA block copolymeric amphiphiles that self-assemble into unilamellar vesicles that can be further oxidatively destabilized. We selected poly(ethylene glycol) (PEG) as the hydrophilic A blocks, owing to its resistance to protein adsorption and low toxicity. As hydrophobic B blocks, we selected poly(propylene sulphide) (PPS), owing to its extreme hydrophobicity, its low glass-transition temperature, and most importantly its oxidative conversion from a hydrophobe to a hydrophile, poly(propylene sulphoxide) and ultimately poly(propylene sulphone). This is the first example of the use of oxidative conversions to destabilize such carriers. This new class of oxidation-responsive polymeric vesicles may find applications as nanocontainers in drug delivery, biosensing and biodetection.

Hydrogen Peroxide↗
PubMed2001

Flow injection analysis of L-lactate in milk and yoghurt by on-line microdialysis and amperometric detection at a disposable biosensor.

A disposable lactate biosensor able to operate in flow injection analysis is described and characterized. The biosensing layer, obtained by glutaraldehyde co-crosslinking of lactate oxidase with bovine serum albumin, was cast on an underlying electropolymerized layer of overoxidized polypyrrole. The resulting biosensor was interference-free and showed a K'M value of 2.4 mmol l-1 and a maximum current density of 440 microA cm-2. When integrated in a flow injection analysis system, a sensitivity of 300 +/- 10 nA mmol-1 l, a linear response up to 1 mmol l-1 and detection limits in the low micromolar range were obtained. The introduction of a microdialysis membrane-based sampler reduced the sensitivity to 7.9 +/- 0.2 nA mmol-1 l and extended the linear range up to 50 mmol l-1 lactate. The anti-interference characteristics of the biosensor permitted lactate determination in untreated milk and diluted yoghurt samples.

Animals↗
PubMed2001

Optical biosensors based on Prussian Blue films.

Optical biosensing schemes based on enzymatically modified inorganic/organic transparent films predominately composed of Prussian Blue are demonstrated. The composite film, which is non-electrochemically deposited on a non-conducting support. is used as an optical transducer for flow-through biosensors based on hydrolases and oxidases. Urease and glucose oxidase are utilized as model enzymes. Action of the urea biosensor is based on optical pH sensitivity of Prussian Blue indicator. The glucose biosensor is acting as first-generation optical biosensor based on in situ generated Prussian White transducer for hydrogen peroxide. These simple, single-pass transmission optical biosensors exhibit sensitivity in the millimolar range of concentration. The biosensors are very stable owing to presence of a poly(pyrrolylbenzoic acid) network in the composite material. This organic polymer plays a dual role as a binding agent for inorganic material and as a functionalized support for strong covalent immobilization of enzyme molecules.

Journal Article↗