Room-Temperature Optical Picocavities below 1 nm<sup>3</sup> Accessing Single-Atom Geometries.
de Nijs, Bart
The journal of physical chemistry letters
American Chemical Society (ACS)
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Carnegie, C., Griffiths, J., de Nijs, B., Readman, C., Chikkaraddy, R., Deacon, W., Zhang, Y., et al. (2018). Room-Temperature Optical Picocavities below 1 nm<sup>3</sup> Accessing Single-Atom Geometries.. The journal of physical chemistry letters, 9 (24), 7146-7151. https://doi.org/10.1021/acs.jpclett.8b03466
Reproducible confinement of light at the nanoscale is essential for the ability to observe and control chemical reactions at the single-molecule level. Here we reliably form millions of identical nanocavities and show that the light can be further focused down to the sub-nanometre scale via the creation of picocavities - single adatom protrusions with angstrom-level resolution. For the first time we stabilise and analyse these cavities at room temperatures through high-speed surface enhanced Raman on specifically selected molecular components, collecting and analysing more than 2 million spectra. Data obtained on these picocavities allows us to deduce structural information on the nanoscale, showing that thiol binding to gold destabilises the metal surface to optical irradiation. Nitrile moieties are found to stabilise picocavities by ten-fold against their disappearance, surviving typically for more than 1s. Such constructs demonstrate the accessibility of single molecule chemistry under ambient conditions.
European Commission Horizon 2020 (H2020) ERC (778616)
Isaac Newton Trust (18.08(K))
Leverhulme Trust (ECF-2018-021)
External DOI: https://doi.org/10.1021/acs.jpclett.8b03466
This record's URL: https://www.repository.cam.ac.uk/handle/1810/287344