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Plasmonic tunnel junctions for single-molecule redox chemistry

Author

Listed:
  • Bart Nijs

    (University of Cambridge)

  • Felix Benz

    (University of Cambridge)

  • Steven J. Barrow

    (University of Cambridge)

  • Daniel O. Sigle

    (University of Cambridge)

  • Rohit Chikkaraddy

    (University of Cambridge)

  • Aniello Palma

    (University of Cambridge)

  • Cloudy Carnegie

    (University of Cambridge)

  • Marlous Kamp

    (University of Cambridge)

  • Ravishankar Sundararaman

    (Rensselaer Polytechnic Institute)

  • Prineha Narang

    (Harvard University)

  • Oren A. Scherman

    (University of Cambridge)

  • Jeremy J. Baumberg

    (University of Cambridge)

Abstract

Nanoparticles attached just above a flat metallic surface can trap optical fields in the nanoscale gap. This enables local spectroscopy of a few molecules within each coupled plasmonic hotspot, with near thousand-fold enhancement of the incident fields. As a result of non-radiative relaxation pathways, the plasmons in such sub-nanometre cavities generate hot charge carriers, which can catalyse chemical reactions or induce redox processes in molecules located within the plasmonic hotspots. Here, surface-enhanced Raman spectroscopy allows us to track these hot-electron-induced chemical reduction processes in a series of different aromatic molecules. We demonstrate that by increasing the tunnelling barrier height and the dephasing strength, a transition from coherent to hopping electron transport occurs, enabling observation of redox processes in real time at the single-molecule level.

Suggested Citation

  • Bart Nijs & Felix Benz & Steven J. Barrow & Daniel O. Sigle & Rohit Chikkaraddy & Aniello Palma & Cloudy Carnegie & Marlous Kamp & Ravishankar Sundararaman & Prineha Narang & Oren A. Scherman & Jeremy, 2017. "Plasmonic tunnel junctions for single-molecule redox chemistry," Nature Communications, Nature, vol. 8(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_s41467-017-00819-7
    DOI: 10.1038/s41467-017-00819-7
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