Plasmonic tunnel junctions for single-molecule redox chemistry
| Autor: | de Nijs, Bart, Benz, Felix, Barrow, Steven J., Sigle, Daniel O., Chikkaraddy, Rohit, Palma, Aniello, Carnegie, Cloudy, Kamp, Marlous, Sundararaman, Ravishankar, Narang, Prineha, Scherman, Oren A., Baumberg, Jeremy J. |
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| Přispěvatelé: | Chikkaraddy, Rohit [0000-0002-3840-4188], Kamp, Marlous [0000-0003-4915-1312], Scherman, Oren [0000-0001-8032-7166], Baumberg, Jeremy [0000-0002-9606-9488], Apollo - University of Cambridge Repository |
| Jazyk: | angličtina |
| Rok vydání: | 2017 |
| Předmět: | |
| Zdroj: | Nature Communications, Vol 8, Iss 1, Pp 1-8 (2017) Nature Communications |
| ISSN: | 2041-1723 |
| Popis: | 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. Plasmons in sub-nm cavities can enable chemical processes within plasmonic hotspots. Here the authors use surface-enhanced Raman spectroscopy to track hot-electron-induced chemical reduction processes in aromatic molecules, thus enabling observation of redox processes at the single-molecule level. |
| Databáze: | OpenAIRE |
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