Publications

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A magnetically active Fe3O4/poly(ethylene oxide)-block-poly(butadiene) (PEO-b-PBD) nanocomposite is formed by the encapsulation of magnetite nanoparticles with a short-chain amphiphilic block copolymer. This material is then incorporated into the self-assembly of higher order polymer architectures, along with an organic pigment, to yield biosynthetic, bifunctional optical and magnetically active Fe3O4/bacteriochlorophyll c/PEO-b-PBD polymeric chlorosomes.

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Core–shell nanostructures are promising candidates for the next generation of catalysts due to synergistic effects which can arise from having two active species in close contact, leading to increased activity. Likewise, catalysts displaying added functionality, such as a magnetic response, can have increased scientific and industrial potential. Here, Pd/Fe3O4 core–shell nanowire clusters are synthesized and applied as hydrogenation catalysts for an industrially important hydrogenation reaction: the conversion of acetophenone to 1-phenylethanol. During synthesis, the palladium nanowires self-assemble into clusters which act as a high-surface-area framework for the growth of a magnetic iron oxide shell. This material demonstrates excellent catalytic activity due to the presence of palladium while the strong magnetic properties provided by the iron oxide shell enable facile catalyst recovery.

Extensive study of photorefractive polymeric composites photosensitized with semiconductor nanocrystals has yielded data indicating that the inclusion of such nanocrystals enhances the charge-carrier mobility, and subsequently leads to a reduction in the photorefractive response time. Unfortunately, the included nanocrystals may also act as a source of deep traps, resulting in diminished diffraction efficiencies as well as reduced two beam coupling gain coefficients. Nonetheless, previous studies indicate that this problem is mitigated through the inclusion of semiconductor nanocrystals possessing a relatively narrow band-gap. Here, we fully exploit this property by doping PbS nanocrystals into a newly formulated photorefractive composite based on molecular triphenyldiamine photosensitized with C60. Through this approach, response times of 399 μs are observed, opening the door for video and other high-speed applications. It is further demonstrated that this improvement in response time occurs with little sacrifice in photorefractive efficiency, with internal diffraction efficiencies of 72% and two-beam-coupling gain coefficients of 500 cm-1 being measured. A thorough analysis of the experimental data is presented, supporting the hypothesized mechanism of enhanced charge mobility without the accompaniment of superfluous traps. It is anticipated that this approach can play a significant role in the eventual commercialization of this class of materials.

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Ternary polymer brushes consisting of polystyrene, poly(methyl methacrylate), and poly(4-vinylpyridine) have been synthesized. These brushes laterally phase separate into several distinct phases and can be tailored by altering the relative polymer composition. Self-consistent field theory has been used to predict the phase diagram and model both the horizontal and vertical phase behavior of the polymer brushes. All phase behaviors observed experimentally correlate well with the theoretical model.

Magnetic nanoparticles are the next tool in medical diagnoses and treatment in many different biomedical applications, including magnetic hyperthermia as alternative treatment for cancer and bacterial infections, as well as the disruption of biofilms. The colloidal stability of the magnetic nanoparticles in a biological environment is crucial for efficient delivery. A surface that can be easily modifiable can also improve the delivery and imaging properties of the magnetic nanoparticle by adding targeting and imaging moieties, providing a platform for additional modification. The strategy presented in this work includes multiple nitroDOPA anchors for robust binding to the surface tied to the same polymer backbone as multiple poly(ethylene oxide) chains for steric stability. This approach provides biocompatibility and enhanced stability in fetal bovine serum (FBS) and phosphate buffer saline (PBS). As a proof of concept, these polymer-particles complexes were then modified with a near infrared dye and utilized in characterizing the integration of magnetic nanoparticles in biofilms. The work presented in this manuscript describes the synthesis and characterization of a nontoxic platform for the labeling of near IR-dyes for bioimaging.

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The synthesis of well-defined nanoparticle materials has been an area of intense investigation, but size control in nanoparticle syntheses is largely empirical. Here, we introduce a general method for fine size control in the synthesis of nanoparticles by establishing steady state growth conditions through the continuous, controlled addition of precursor, leading to a uniform rate of particle growth. This approach, which we term the "xtended LaMer mechanism" allows for reproducibility in particle size from batch to batch as well as the ability to predict nanoparticle size by monitoring the early stages of growth. We have demonstrated this method by applying it to a challenging synthetic system: magnetite nanoparticles. To facilitate this reaction, we have developed a reproducible method for synthesizing an iron oleate precursor that can be used without purification. We then show how such fine size control affects the performance of magnetite nanoparticles in magnetic hyperthermia.

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The photosensitization of photorefractive polymeric composites for operation at 633 nm is accomplished through the inclusion of narrow band gap semiconductor nanocrystals composed of PbS. Unlike previous studies involving photosensitization of photorefractive polymer composites with inorganic nanocrystals, we employ an off-resonance approach where the first excitonic transition associated with the PbS nanocrystals lies at ∼1220 nm and not the wavelength of operation. Using this methodology, internal diffraction efficiencies exceeding 82%, two-beam-coupling gain coefficients of 211 cm^-1, and response times of 34 ms have been observed, representing some of the best figures of merit reported for this class of materials. These data demonstrate the ability of semiconductor nanocrystals to compete effectively with traditional organic photosensitizers. In addition to superior performance, this approach also offers an inexpensive and easy means by which to photosensitize composite materials. The photoconductive characteristics of the composites used for this study will also be considered.

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