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Plasmonic tunnel junctions for single-molecule redox chemistry

de Nijs, Bart, Benz, Felix, Barrow, Steven J., Sigle, Daniel O., Chikkaraddy, Rohit, Palma, Aniello, Carnegie, Cloudy, Kamp, Marlous, Sundararaman, Ravishankar, Narang, Prineha, and others. (2017) Plasmonic tunnel junctions for single-molecule redox chemistry. Nature Communications, 8 . ISSN 2041-1723. (doi:10.1038/s41467-017-00819-7) (KAR id:64608)

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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.

Item Type: Article
DOI/Identification number: 10.1038/s41467-017-00819-7
Subjects: Q Science > QC Physics > QC176.8.N35 Nanoscience, nanotechnology
Q Science > QC Physics > QC355 Optics
Q Science > QD Chemistry > QD431 Organic Chemistry- Biochemistry- Proteins, peptides, amino acids
Divisions: Divisions > Division of Natural Sciences > Physics and Astronomy
Depositing User: Aniello Palma
Date Deposited: 22 Nov 2017 11:13 UTC
Last Modified: 09 Dec 2022 05:24 UTC
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