Room-Temperature Optical Picocavities below 1 nm3 Accessing Single-Atom Geometries
| Autor: | Charlie Readman, István Szabó, Cloudy Carnegie, Jeremy J. Baumberg, Rohit Chikkaraddy, Javier Aizpurua, Yao Zhang, Bart de Nijs, William M. Deacon, Edina Rosta, Jack Griffiths |
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| Přispěvatelé: | Engineering and Physical Sciences Research Council (UK), Isaac Newton Trust, Leverhulme Trust, Trinity College Dublin, Chikkaraddy, Rohit [0000-0002-3840-4188], Szabó, István [0000-0002-3700-3614], Rosta, Edina [0000-0002-9823-4766], Aizpurua, Javier [0000-0002-1444-7589], Baumberg, Jeremy J [0000-0002-9606-9488], Apollo - University of Cambridge Repository |
| Rok vydání: | 2018 |
| Předmět: |
0306 Physical Chemistry (incl. Structural)
Materials science 0299 Other Physical Sciences Atom (order theory) 02 engineering and technology 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences Chemical reaction 0104 chemical sciences Chemical physics General Materials Science Physical and Theoretical Chemistry 0210 nano-technology |
| Zdroj: | Digital.CSIC. Repositorio Institucional del CSIC instname |
| DOI: | 10.17863/cam.34648 |
| Popis: | Reproducible confinement of light on 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 subnanometer scale via the creation of picocavities, single-adatom protrusions with angstrom-level resolution. For the first time, we stabilize and analyze these cavities at room temperatures through high-speed surface-enhanced Raman spectroscopy on specifically selected molecular components, collecting and analyzing 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 destabilizes the metal surface to optical irradiation. Nitrile moieties are found to stabilize picocavities by 10-fold against their disappearance, typically surviving for >1 s. Such constructs demonstrate the accessibility of single-molecule chemistry under ambient conditions. We acknowledge financial support from EPSRC Grants EP/L027151/1 and EP/N020669/1. C.C. acknowledges support from NPL PO443073. B.d.N. acknowledges support from the Leverhulme Trust and Isaac Newton Trust. R.C. acknowledges financial support from a Junior Research Fellowship of Trinity College. |
| Databáze: | OpenAIRE |
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