School of Chemistry - Research Publications

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Start date: 2000 × Author: Davis, Timothy × Author: Roberts, Ann ×

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    Large-Area Nanofabrication of Partially Embedded Nanostructures for Enhanced Plasmonic Hot-Carrier Extraction
    Ng, C ; Zeng, P ; Lloyd, JA ; Chakraborty, D ; Roberts, A ; Smith, TA ; Bach, U ; Sader, JE ; Davis, TJ ; Gomez, DE (AMER CHEMICAL SOC, 2019-03-01)
    When plasmonic nanoparticles are coupled with semiconductors, highly energetic hot carriers can be extracted from the metal-semiconductor interface for various applications in light energy conversion. However, the current quantum yields for hot-electron extraction are generally low. An approach for increasing the extraction efficiency consists of maximizing the contact area between the surface of the metal nanostructure and the electron-accepting material. In this work, we developed an innovative, simple, and scalable fabrication technique that partially embeds colloidal plasmonic nanostructures within a semiconductor TiO2 layer without utilizing any complex top-down nanofabrication method. The successful embedding is confirmed by scanning electron microscopy and atomic force microscopy imaging. Using visible-pump, near-IR probe transient absorption spectroscopy, we also provide evidence that the increase in the surface contact area between the nanostructures and the electron-accepting material leads to an increase in the amount of hot-electron injection into the TiO2 layer.
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    Luminescence of a Transition Metal Complex Inside a Metamaterial Nanocavity
    Connell, TU ; Earl, SK ; Ng, C ; Roberts, A ; Davis, TJ ; White, JM ; Polyzos, A ; Gomez, DE (John Wiley & Sons, 2017-08-25)
    Modification of the local density of optical states using metallic nanostructures leads to enhancement in the number of emitted quanta and photocatalytic turnover of luminescent materials. In this work, the fabrication of a metamaterial is presented that consists of a nanowire separated from a metallic mirror by a polymer thin film doped with a luminescent organometallic iridium(III) complex. The large spin–orbit coupling of the heavy metal atom results in an excited state with significant magnetic-dipole character. The nanostructured architecture supports two distinct optical modes and their assignment achieved with the assistance of numerical simulations. The simulations show that one mode is characterized by strong confinement of the electric field and the other by strong confinement of the magnetic field. These modes elicit drastic changes in the emitter’s photophysical properties, including dominant nanocavity-derived modes observable in the emission spectra along with significant increases in emission intensity and the total decay rate. A combination of simulations and momentum-resolved spectroscopy helps explain the mechanism of the different interactions of each optical mode supported by the metamaterial with the excited state of the emitter.
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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.