Dynamics of deterministically positioned single‐bond surface‐enhanced Raman scattering from DNA origami assembled in plasmonic nanogaps

Rohit Chikkaraddy; Vladimir A Turek; Qianqi Lin; Jack Griffiths; Bart Nijs; Ulrich F Keyser; Jeremy J Baumberg

doi:10.1002/jrs.5997

Dynamics of deterministically positioned single‐bond surface‐enhanced Raman scattering from DNA origami assembled in plasmonic nanogaps

Rohit Chikkaraddy, Vladimir A Turek, Qianqi Lin, Jack Griffiths, Bart Nijs, Ulrich F Keyser, Jeremy J Baumberg

Physics and Astronomy

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Abstract

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 are precisely controlled using DNA origami constructs. The observed SERS intensities and 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 reveal significant modifications to bond vibrations and selection rules over time.

Original language	English
Pages (from-to)	348-354
Journal	Journal of Raman Spectroscopy
Volume	52
Issue number	2
Early online date	30 Sept 2020
DOIs	https://doi.org/10.1002/jrs.5997
Publication status	Published - Feb 2021

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title = "Dynamics of deterministically positioned single‐bond surface‐enhanced Raman scattering from DNA origami assembled in plasmonic nanogaps",

abstract = "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 are precisely controlled using DNA origami constructs. The observed SERS intensities and 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 reveal significant modifications to bond vibrations and selection rules over time.",

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T1 - Dynamics of deterministically positioned single‐bond surface‐enhanced Raman scattering from DNA origami assembled in plasmonic nanogaps

AU - Chikkaraddy, Rohit

AU - Turek, Vladimir A

AU - Lin, Qianqi

AU - Griffiths, Jack

AU - Nijs, Bart

AU - Keyser, Ulrich F

AU - Baumberg, Jeremy J

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N2 - 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 are precisely controlled using DNA origami constructs. The observed SERS intensities and 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 reveal significant modifications to bond vibrations and selection rules over time.

AB - 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 are precisely controlled using DNA origami constructs. The observed SERS intensities and 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 reveal significant modifications to bond vibrations and selection rules over time.

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JF - Journal of Raman Spectroscopy

IS - 2

ER -

Dynamics of deterministically positioned single‐bond surface‐enhanced Raman scattering from DNA origami assembled in plasmonic nanogaps

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