Plasmonic tunnel junctions for single-molecule redox chemistry

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 and Jeremy J. Baumberg ()
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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

Nature Communications, 2017, vol. 8, issue 1, 1-8

Abstract: 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.

Date: 2017
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DOI: 10.1038/s41467-017-00819-7

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