School of Physics - Research Publications

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Author: Roberts, Ann × Author: Gomez, Daniel × Author: Cadusch, Jasper × End date: 2018 × Start date: 2010 ×

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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.
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    Photoinduced Electron Transfer in the Strong Coupling Regime: Waveguide-Plasmon Polaritons
    Zeng, P ; Cadusch, J ; Chakraborty, D ; Smith, TA ; Roberts, A ; Sader, JE ; Davis, TJ ; Gomez, DE (AMER CHEMICAL SOC, 2016-04)
    Reversible exchange of photons between a material and an optical cavity can lead to the formation of hybrid light-matter states where material properties such as the work function [ Hutchison et al. Adv. Mater. 2013 , 25 , 2481 - 2485 ], chemical reactivity [ Hutchison et al. Angew. Chem., Int. Ed. 2012 , 51 , 1592 - 1596 ], ultrafast energy relaxation [ Salomon et al. Angew. Chem., Int. Ed. 2009 , 48 , 8748 - 8751 ; Gomez et al. J. Phys. Chem. B 2013 , 117 , 4340 - 4346 ], and electrical conductivity [ Orgiu et al. Nat. Mater. 2015 , 14 , 1123 - 1129 ] of matter differ significantly to those of the same material in the absence of strong interactions with the electromagnetic fields. Here we show that strong light-matter coupling between confined photons on a semiconductor waveguide and localized plasmon resonances on metal nanowires modifies the efficiency of the photoinduced charge-transfer rate of plasmonic derived (hot) electrons into accepting states in the semiconductor material. Ultrafast spectroscopy measurements reveal a strong correlation between the amplitude of the transient signals, attributed to electrons residing in the semiconductor and the hybridization of waveguide and plasmon excitations.
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    Hot Carrier Extraction with Plasmonic Broadband Absorbers
    Ng, C ; Cadusch, JJ ; Dligatch, S ; Roberts, A ; Davis, TJ ; Mulvaney, P ; Gomez, DE (American Chemical Society, 2016-04-01)
    Hot charge carrier extraction from metallic nanostructures is a very promising approach for applications in photocatalysis, photovoltaics, and photodetection. One limitation is that many metallic nanostructures support a single plasmon resonance thus restricting the light-to-charge-carrier activity to a spectral band. Here we demonstrate that a monolayer of plasmonic nanoparticles can be assembled on a multistack layered configuration to achieve broadband, near-unit light absorption, which is spatially localized on the nanoparticle layer. We show that this enhanced light absorbance leads to ∼40-fold increases in the photon-to-electron conversion efficiency by the plasmonic nanostructures. We developed a model that successfully captures the essential physics of the plasmonic hot electron charge generation and separation in these structures. This model also allowed us to establish that efficient hot carrier extraction is limited to spectral regions where (i) the photons have energies higher than the Schottky junctions and (ii) the absorption of light is localized on the metal nanoparticles.