School of Physics - Research Publications
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ItemDirect Assembly of Large Area Nanoparticle Arrays(AMER CHEMICAL SOC, 2018-08-01)A major goal of nanotechnology is the assembly of nanoscale building blocks into functional optical, electrical, or chemical devices. Many of these applications depend on an ability to optically or electrically address single nanoparticles. However, positioning large numbers of single nanocrystals with nanometer precision on a substrate for integration into solid-state devices remains a fundamental roadblock. Here, we report fast, scalable assembly of thousands of single nanoparticles using electrophoretic deposition. We demonstrate that gold nanospheres down to 30 nm in size and gold nanorods <100 nm in length can be assembled into predefined patterns on transparent conductive substrates within a few seconds. We find that rod orientation can be preserved during deposition. As proof of high fidelity scale-up, we have created centimeter scale patterns comprising more than 1 million gold nanorods.
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ItemTuning of Plasmonic Resonances in the Near Infrared Spectrum Using a Double Coaxial Aperture Array(IEEE-INST ELECTRICAL ELECTRONICS ENGINEERS INC, 2018-12-01)
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ItemDirected Chemical Assembly of Single and Clustered Nanoparticles with Silanized Templates(AMER CHEMICAL SOC, 2018-06-26)The assembly of nanoscale materials into arbitrary, organized structures remains a major challenge in nanotechnology. Herein, we report a general method for creating 2D structures by combining top-down lithography with bottom-up chemical assembly. Under optimal conditions, the assembly of gold nanoparticles was achieved in less than 30 min. Single gold nanoparticles, from 10 to 100 nm, can be placed in predetermined patterns with high fidelity, and higher-order structures can be generated consisting of dimers or trimers. It is shown that the nanoparticle arrays can be transferred to, and embedded within, polymer films. This provides a new method for the large-scale fabrication of nanoparticle arrays onto diverse substrates using wet chemistry.
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ItemDirect Assembly of Large Area Nanoparticle Arrays( 2018-07-13)We describe the fabrication of large area arrays of single nanoparticles using electrophoretic deposition.
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ItemHot-Carrier Organic Synthesis via the Near-Perfect Absorption of Light(AMER CHEMICAL SOC, 2018-11-01)Photocatalysis enables the synthesis of valuable organic compounds by exploiting photons as a chemical reagent. Although light absorption is an intrinsic step, existing approaches rely on poorly absorbing catalysts that require high illumination intensities to afford enhanced efficiencies. Here, we demonstrate that a plasmonic metamaterial capable of near-perfect light absorption (94%) readily catalyzes a model organic reaction with a 29-fold enhancement in conversion relative to controls. The oxidation of benzylamine proceeds via a reactive iminium intermediate with high selectivity at ambient temperature and pressure, using only low-intensity visible irradiation. Control experiments demonstrated that only hot charge carriers produced following photoexcitation facilitate the formation of superoxide radicals, which, in turn, leads to iminium formation. Modeling shows that hot holes with energies that overlap with the highest-occupied molecular orbital (HOMO) of the reactant can participate and initiate the photocatalytic conversion. These results have important implications for hot-carrier photocatalysis and plasmon-hot-carrier extraction.
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ItemOptical image processing with metasurface dark modes(OPTICAL SOC AMER, 2018-09-01)Here we consider image processing using the optical modes of metasurfaces with an angle-dependent excitation. These spatially dispersive modes can be used to directly manipulate the spatial frequency content of an incident field, suggesting their use as ultra-compact alternatives for analog optical information processing. A general framework for describing the filtering process in terms of the optical transfer functions is provided. In the case where the relevant mode cannot be excited with a normally incident plane wave (a dark mode), high-pass filtering is obtained. We provide examples demonstrating filtering of both amplitude and pure phase objects.
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ItemMetasurfaces, dark modes, and high NA illumination(OPTICAL SOC AMER, 2018-10-15)The interaction of a focused beam with a metasurface supporting dark modes is investigated. We show computationally and experimentally that the excitation of dark modes is accompanied by characteristic changes in the reflected Fourier spectrum. This spatial frequency filtering capability indicates an avenue for the all-optical, on-chip detection of phase gradients for biological and other imaging techniques.
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ItemCathodoluminescence as a probe of the optical properties of resonant apertures in a metallic film(BEILSTEIN-INSTITUT, 2018-05-18)Here we present the results of an investigation of resonances of azimuthal trimer arrangements of rectangular slots in a gold film on a glass substrate using cathodoluminescence (CL) as a probe. The variation in the CL signal collected from specific locations on the sample as a function of wavelength and the spatial dependence of emission into different wavelength bands provides considerable insight into the resonant modes, particularly sub-radiant modes, of these apertures. By comparing our experimental results with electromagnetic simulations we are able to identify a Fabry-Pérot mode of these cavities as well as resonances associated with the excitation of surface plasmon polaritons on the air-gold boundary. We obtain evidence for the excitation of dark (also known as sub-radiant) modes of apertures and aperture ensembles.
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