Dynamics of Deterministically-Positioned Single-Bond SERS from DNA Origami Assembled in Plasmonic Nanogaps
de Nijs, Bart
Journal of Raman Spectroscopy
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Chikkaraddy, R., Turek, V., Lin, Q., Griffiths, J., de Nijs, B., Keyser, U., & Baumberg, J. Dynamics of Deterministically-Positioned Single-Bond SERS from DNA Origami Assembled in Plasmonic Nanogaps. Journal of Raman Spectroscopy https://doi.org/10.17863/CAM.57134
We study the dynamics of single bonds through the surface enhanced Raman scattering (SERS) from single SERS-marker molecules containing a distinctive single alkyl bond. Assembly of the nanogaps and positioning of single molecules inside the electromagnetic hotspot is precisely controlled using DNA origami constructs. The observed SERS intensities, their spectral wandering, together with electromagnetic simulations, all confirm the role of picocavities in this nanogap geometry in allowing observation of SERS signatures from individual vibrating bonds. The strong electromagnetic field around each picocavity and the transient binding of the SERS-marker molecule reveals significant modifications to bond vibrations and selection rules over time.
Support from Trinity College, University of Cambridge and Leverhulme Trust and Isaac Newton Trust in the form of an Early Career Fellowships.
Isaac Newton Trust (18.08(K))
Leverhulme Trust (ECF-2018-021)
EPSRC (via University of Exeter) (EP/R020965/1)
European Commission Horizon 2020 (H2020) Future and Emerging Technologies (FET) (829067)
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This record's DOI: https://doi.org/10.17863/CAM.57134
This record's URL: https://www.repository.cam.ac.uk/handle/1810/310045
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