Mid-infrared-perturbed molecular vibrational signatures in plasmonic nanocavities

Rohit Chikkaraddy; Angelos Xomalis; Lukas A. Jakob; Jeremy J. Baumberg

doi:10.1038/s41377-022-00709-8

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Mid-infrared-perturbed molecular vibrational signatures in plasmonic nanocavities

Articles

- Mid-infrared-perturbed molecular vibrational signatures in plasmonic nanocavities
- Light: Science & Applications Vol. 11, Issue 1, Pages: 127-135(2022)
- Affiliations：
  
  1.NanoPhotonics Centre, Cavendish Laboratory, Department of Physics, JJ Thompson Avenue, University of Cambridge, Cambridge, CB3 0HE, UK
  2.Present address: Empa, Swiss Federal Laboratories for Materials Science and Technology, Laboratory for Mechanics of Materials and Nanostructures, Thun, Switzerland
- Author bio：
  
  Rohit Chikkaraddy (rc621@cam.ac.uk)
  Jeremy J. Baumberg (jjb12@cam.ac.uk)
- Funds：
- DOI：10.1038/s41377-022-00709-8
  CLC：
- Published：31 January 2022，
  
  Published Online：19 January 2022，
  
  Received：12 July 2021，
  
  Revised：15 November 2021，
  
  Accepted：05 January 2022
- Accepted：
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Chikkaraddy, R. et al. Mid-infrared-perturbed molecular vibrational signatures in plasmonic nanocavities. Light: Science & Applications, 11, 127-135 (2022).
DOI：

Chikkaraddy, R. et al. Mid-infrared-perturbed molecular vibrational signatures in plasmonic nanocavities. Light: Science & Applications, 11, 127-135 (2022). DOI： 10.1038/s41377-022-00709-8.

摘要

Abstract

Recent developments in surface-enhanced Raman scattering (SERS) enable observation of single-bond vibrations in real time at room temperature. By contrast

mid-infrared (MIR) vibrational spectroscopy is limited to inefficient slow detection. Here we develop a new method for MIR sensing using SERS. This method utilizes nanoparticle-on-foil (NPoF) nanocavities supporting both visible and MIR plasmonic hotspots in the same nanogap formed by a monolayer of molecules. Molecular SERS signals from individual NPoF nanocavities are modulated in the presence of MIR photons. The strength of this modulation depends on the MIR wavelength

and is maximized at the 6–12 μm absorption bands of SiO

or polystyrene placed under the foil. Using a single-photon lock-in detection scheme we time-resolve the rise and decay of the signal in a few 100 ns. Our observations reveal that the phonon resonances of SiO

can trap intense MIR surface plasmons within the Reststrahlen band

tuning the visible-wavelength localized plasmons by reversibly perturbing the localized few-nm-thick water shell trapped in the nanostructure crevices. This suggests new ways to couple nanoscale bond vibrations for optomechanics

with potential to push detection

limits down to single-photon and single-molecule regimes.

关键词

Keywords

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