Locating Single-Atom Optical Picocavities Using Wavelength-Multiplexed Raman Scattering.
American Chemical Society (ACS)
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Griffiths, J., de Nijs, B., Chikkaraddy, R., & Baumberg, J. J. (2021). Locating Single-Atom Optical Picocavities Using Wavelength-Multiplexed Raman Scattering.. ACS Photonics, 8 (10), 2868-2875. https://doi.org/10.1021/acsphotonics.1c01100
Funder: Leverhulme Trust
Funder: Trinity College, University of Cambridge
Funder: Isaac Newton Trust
Transient atomic protrusions in plasmonic nanocavities confine optical fields to sub-1-nm3 picocavities, allowing the optical interrogation of single molecules at room temperature. While picocavity formation is linked to both the local chemical environment and optical irradiation, the role of light in localizing the picocavity formation is unclear. Here, we combine information from thousands of picocavity events and simultaneously compare the transient Raman scattering arising from two incident pump wavelengths. Full analysis of the data set suggests that light suppresses the local effective barrier height for adatom formation and that the initial barrier height is decreased by reduced atomic coordination numbers near facet edges. Modeling the system also resolves the frequency-dependent picocavity field enhancements supported by these atomic scale features.
European Research Council (ERC) under Horizon 2020 research and innovation programme PICOFORCE (Grant Agreement No. 883703) and POSEIDON (Grant Agreement No. 861950). We acknowledge funding from the EPSRC (Cambridge NanoDTC EP/L015978/1, EP/L027151/1, EP/S022953/1, EP/P029426/1, and EP/R020965/1.
Isaac Newton Trust (18.08(K))
Leverhulme Trust (ECF-2018-021)
Engineering and Physical Sciences Research Council (EP/L027151/1)
European Commission Horizon 2020 (H2020) Research Infrastructures (RI) (861950)
European Commission Horizon 2020 (H2020) ERC (883703)
Engineering and Physical Sciences Research Council (EP/L015978/1)
Engineering and Physical Sciences Research Council (EP/P029426/1)
Engineering and Physical Sciences Research Council (EP/R020965/1)
Engineering and Physical Sciences Research Council (EP/S022953/1)
External DOI: https://doi.org/10.1021/acsphotonics.1c01100
This record's URL: https://www.repository.cam.ac.uk/handle/1810/332159
Attribution 4.0 International
Licence URL: https://creativecommons.org/licenses/by/4.0/