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Biomedical subjects

T Andrew Taton

Publications and source records attributed to T Andrew Taton.

13 recordsLinked to original sources

DNA dissociation and degradation at gold nanoparticle surfaces.

The instability of DNA-functionalized gold nanoparticles (Au-DNA conjugates) upon exposure to high temperatures is characterized using fluorescence spectroscopy, gel electrophoresis and ion-exchange chromatography. Above 70 degrees C, aqueous Au-DNA conjugates decompose within hours due to both desorption of thiol-terminated DNA from the gold nanoparticle surface and chemical degradation of DNA in the presence of colloidal gold. Although the chemical mechanism for DNA degradation was not identified in this study, the gold surface participates directly in the cleavage reaction. These results have important implications for the use of Au-DNA conjugates in biotechnological and clinical applications that require high temperatures, such as polymerase chain reaction (PCR).

Chromatography, High Pressure Liquid↗

Plasmonic nanoparticle chains via a morphological, sphere-to-string transition.

Au nanoparticles encapsulated within polystyrene-block-poly(acrylic acid) (PS-b-PAA) micelles assemble into regular, one-dimensional arrays when they are exposed to solvent conditions that relax interfacial curvature in the micellar shell. Nanoparticle chaining was induced by adding salt, acid, or cationic carbodiimide to the suspension of purified encapsulated Au nanoparticles (Au@PS-b-PAA). The resulting assemblies were characterized by scanning and transmission electron microscopies, by dark-field optical microscopy, and by visible absorption spectroscopy. The length of the chains was modulated by varying the concentration of additive. More importantly, the spacing between Au nanoparticles was dictated entirely by the shell thickness of the Au@PS-b-PAA starting material. Far-field polarization microspectroscopy demonstrated directional surface plasmon coupling in a straightened nanoparticle chain, which is a basic requirement for the use of these assemblies as plasmon waveguides.

Acrylic Resins↗

Thermal transport in au-core polymer-shell nanoparticles.

Thermal transport in aqueous suspensions of Au-core polymer-shell nanoparticles is investigated by time-resolved measurements of optical absorption. The addition of an organic cosolvent to the suspension causes the polystyrene component of the polymer shell to swell, and this change in the microstructure of the shell increases the effective thermal conductivity of the shell by a factor of approximately 2. The corresponding time scale for the cooling of the nanoparticle decreases from 200 ps to approximately 100 ps. The threshold concentration of cosolvent that creates the changes in thermal conductivity, 5 vol % tetrahydrofuran in water or 40 vol % N,N-dimethylformamide in water, is identical to the threshold concentrations for producing small shifts in the frequency of the plasmon resonance. Because the maximum fraction of solvent in the polymer shell is less than 20 vol %, the increase in the effective thermal conductivity of the shell cannot be easily explained by contributions to heat transport by the solvent or enhanced alignment of the polystyrene backbone along the radial direction.

Gold↗

Magnetomicelles: composite nanostructures from magnetic nanoparticles and cross-linked amphiphilic block copolymers.

We report the synthesis, characterization, and covalent surface chemistry of "magnetomicelles", cross-linked, amphiphilic block-copolymer micelles that encapsulate superparamagnetic iron oxide nanoparticles. Because these composite nanostructures assemble spontaneously from solution by simultaneous desolvation of nanoparticle and amphiphilic poly(styrene(250)-block-acrylic acid(13)) components, explicit surface functionalization of the particles is not required, and the encapsulation method was applied to different magnetic nanoparticle sizes and compositions. TEM images of the magnetomicelles illustrated that the number of encapsulated particles could be dictated rationally by synthetic conditions. The magnetic properties of the particles were characterized by SQUID magnetometry and followed the general Langevin magnetic model for superparamagnetic materials. The micellar shells of these particles were functionalized using covalent chemistry that would not ordinarily be possible on the magnetic particle surface. As a result, this noncovalent approach provides a new route to technological applications of hydrophobic magnetic nanomaterials that lack appropriate conjugate surface chemistry.

Journal Article↗

Sequence-encoded self-assembly of multiple-nanocomponent arrays by 2D DNA scaffolding.

Regular 2D arrays of multiple types of nanocomponents were constructed by self-assembly to DNA scaffolding with alternating rows of sequence-encoded hybridization sites. Different-sized Au particles coated with DNA complementary to one of the sites were bound to the scaffolding, producing alternating rows of the two nanocomponents with a 32-nm inter-row spacing. These results demonstrate the potential for using DNA to self-assemble complex arrays of components with nanometer-scale precision.

Base Sequence↗

Micelle-encapsulated carbon nanotubes: a route to nanotube composites.

We report a general approach toward dispersing single-walled carbon nanotubes (SWNTs) in solvents and polymer materials, by encapsulating SWNTs within cross-linked micelles. Micelles made from polystyrene-block-poly(acrylic acid) (PS-b-PAA), an amphiphilic block copolymer, are first assembled around SWNTs by gradually adding H2O to a suspension of nanotubes in dimethylformamide. The hydrophilic, outer shells of these micelles are then chemically cross-linked with a difunctional linker molecule. Pure encapsulated SWNTs (e-SWNTs) can then be separated from empty cross-linked micelles by consecutive cycles of centrifugation and redispersion. Atomic force and transmission electron microscopies of the resulting nanostructures demonstrate that individual nanotubes (rather than bundles) have been completely encased in polymer shells whose thickness is slightly larger than that of empty micelles. e-SWNTs encapsulated in PS-b-PAA can be permanently redispersed in H2O, in organic solvents, and in both hydrophobic and hydrophilic polymer matrices with minimal sonication. Micelle encapsulation could improve the compositing of SWNTs in a wide variety of polymer materials for structural, electronic, and thermal applications.

Journal Article↗

Array-based electrical detection of DNA with nanoparticle probes.

A DNA array detection method is reported in which the binding of oligonucleotides functionalized with gold nanoparticles leads to conductivity changes associated with target-probe binding events. The binding events localize gold nanoparticles in an electrode gap; silver deposition facilitated by these nanoparticles bridges the gap and leads to readily measurable conductivity changes. An unusual salt concentration-dependent hybridization behavior associated with these nanoparticle probes was exploited to achieve selectivity without a thermal-stringency wash. Using this method, we have detected target DNA at concentrations as low as 500 femtomolar with a point mutation selectivity factor of approximately 100,000:1.

Antigens, Bacterial↗

Nanostructures as tailored biological probes.

A new generation of spectroscopic dyes is gradually becoming available to biological researchers, from an unexpected source: materials chemists who study the synthesis and properties of nano-sized inorganic objects. Research into tailoring the optical properties, surface chemistry and biocompatibility of metallic and semiconductor nanoparticles, exemplified in part by a recent report by Mirkin, Schatz and coworkers, is fulfilling the promise of these nanostructures as customizable substitutes for organic molecular probes.

Biosensing Techniques↗

Site-specific, covalent attachment of proteins to a solid surface.

Immobilized and site-specifically labeled proteins are becoming invaluable tools in proteomics. Here, we describe a strategy to attach a desired protein to a solid surface in a covalent, site-specific manner. This approach employs an enzymatic posttranslational modification method to site-specifically label a target protein with an azide; an alternative substrate for protein farnesyl transferase containing an azide group was developed for this purpose. A bio-orthogonal Cu(I)-catalyzed cycloaddition reaction is then used to covalently attach the protein to agarose beads bearing an alkyne functional group. We demonstrate that both the azide incorporation and the capture steps can be performed on either a purified protein target or on a protein present within a complex mixture. This approach involves the use of a four-residue tag which is significantly smaller than most other tags reported to date and results in covalent immobilization of the target protein. Hence it should have significant applicability in protein science.

Base Sequence↗

Encapsulated magnetic nanoparticles as supports for proteins and recyclable biocatalysts.

This paper describes the bioconjugation of histidine-tagged enzymes and other proteins to the surface of composite "magnetomicelles" consisting of magnetic gamma-Fe2O3 nanoparticles encapsulated within cross-linked polystyrene-block-polyacrylate copolymer micelle shells. Free carboxylic acid groups on the magnetomicelle surface were converted to Cu2+-iminodiacetic acid (IDA) for protein capture. The conjugation of T4 DNA ligase and enhanced green fluorescent protein to magnetomicelles revealed that proteins were captured with a high surface density and could be magnetically separated from reaction mixtures and subsequently released from the nanoparticle surface. Additionally, bioconjugation of T7 RNA polymerase yielded a functional enzyme that maintained its biological activity and could be recycled for up to three subsequent transcription reactions. We propose that protein-magnetomicelle bioconjugates are effective for protein bioseparation and enzymatic recycling and further strengthen the idea that nanoparticle surfaces have utility in protein immobilization.

Catalysis↗