Journal
NATURE COMMUNICATIONS
Volume 8, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-017-00819-7
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Funding
- EPSRC [EP/G060649/1, EP/I012060/1, EP/L027151/1]
- ERC grant [LINASS 320503]
- Winton Programme for the Physics of Sustainability
- European Commission for a Marie Curie Fellowship (NANOSPHERE) [658360]
- European Commission for a Marie Curie Fellowship (SPARCLEs) [7020005]
- Harvard University Center for the Environment (HUCE)
- Dr Manmohan Singh scholarship from St John's College
- UK National Physical Laboratories
- Marie Curie Actions (MSCA) [658360] Funding Source: Marie Curie Actions (MSCA)
- Engineering and Physical Sciences Research Council [EP/G060649/1, EP/K028510/1, EP/L027151/1] Funding Source: researchfish
- EPSRC [EP/K028510/1, EP/L027151/1, EP/G060649/1] Funding Source: UKRI
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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.
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