4.7 Article

Electron Transfer and Near-Field Mechanisms in Plasmonic Gold-Nanoparticle-Modified TiO2 Photocatalytic Systems

Journal

ACS APPLIED NANO MATERIALS
Volume 2, Issue 7, Pages 4067-4074

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsanm.9b00485

Keywords

gold; titanium dioxide; surface plasmon resonance (SPR); hot electron; near field; charge transfer; core-shell

Funding

  1. Research Foundation Flanders (FWO)
  2. FWO [G03821SN]
  3. European Research Council (ERC) [335078-COLOURATOM]

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The major mechanism responsible for plasmonic enhancement of titanium dioxide photocatalysis using gold nanoparticles is still under contention. This work introduces an experimental strategy to disentangle the significance of the charge transfer and near-field mechanisms in plasmonic photocatalysis. By controlling the thickness and conductive nature of a nanoparticle shell that acts as a spacer layer separating the plasmonic metal core from the TiO2 surface, field enhancement or charge transfer effects can be selectively repressed or evoked. Layer-by-layer and in situ polymerization methods are used to synthesize gold core polymer shell nanoparticles with shell thickness control up to the sub-nanometer level. Detailed optical and electrical characterization supported by near-field simulation models corroborate the trends in photocatalytic activity of the different systems. This approach mainly points at an important contribution of the enhanced near field.

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