School of Physics - Research Publications

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    Direct Assembly of Large Area Nanoparticle Arrays
    Zhang, H ; Cadusch, J ; Kinnear, C ; James, T ; Roberts, A ; Mulvaney, P (AMER CHEMICAL SOC, 2018-08)
    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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    Directed Chemical Assembly of Single and Clustered Nanoparticles with Silanized Templates
    Kinnear, C ; Cadusch, J ; Zhang, H ; Lu, J ; James, TD ; Roberts, A ; Mulvaney, P (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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    Hot-Carrier Organic Synthesis via the Near-Perfect Absorption of Light
    Xiao, Q ; Connell, TU ; Cadusch, JJ ; Roberts, A ; Chesman, ASR ; Gomez, DE (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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    In-Plane Detection of Guided Surface Plasmons for High-Speed Optoelectronic Integrated Circuits
    Panchenko, E ; Cadusch, JJ ; Avayu, O ; Ellenbogen, T ; James, TD ; Gomez, D ; Roberts, A (WILEY, 2018-01)
    Abstract Constrains on the speed of modern digital integrated circuits are dominated by the metallic interconnects between logic gates. Surface plasmon polaritons have potential to overcome this limitation and greatly increase the operating speed of future digital devices. Nevertheless, an ongoing issue is the compatibility of modern planar microelectronic circuits with current methods for detecting surface plasmons. Here, a new approach to in‐plane surface plasmon polariton detection is proposed and experimentally demonstrated. The design is based on metal–semiconductor–metal photodetectors that are acknowledged as having one of the best speed characteristics among photodetectors. In the design, the photodetector structure also plays a dual role as the outcoupling grating for surface plasmons, significantly reducing the footprint of the resulting device. The technique has the potential to enable the integration of surface plasmons as signal carriers in future high‐speed optoelectronic integrated circuits.