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.
journal_name
Nat Communjournal_title
Nature communicationsauthors
de Nijs B,Benz F,Barrow SJ,Sigle DO,Chikkaraddy R,Palma A,Carnegie C,Kamp M,Sundararaman R,Narang P,Scherman OA,Baumberg JJdoi
10.1038/s41467-017-00819-7subject
Has Abstractpub_date
2017-10-20 00:00:00pages
994issue
1issn
2041-1723pii
10.1038/s41467-017-00819-7journal_volume
8pub_type
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