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  • Featured in Physics
  • Open Access

Raman Probing the Local Ultrastrong Coupling of Vibrational Plasmon Polaritons on Metallic Gratings

Rakesh Arul1, Kishan Menghrajani2, Marie S. Rider2, Rohit Chikkaraddy1, William L. Barnes2,*, and Jeremy J. Baumberg1,†

  • 1NanoPhotonics Centre, Cavendish Laboratory, Department of Physics, JJ Thompson Avenue, University of Cambridge, Cambridge, CB3 0HE, United Kingdom
  • 2Department of Physics and Astronomy, University of Exeter, Exeter, EX4 4QL, United Kingdom

  • *Corresponding author: W.L.Barnes@exeter.ac.uk
  • †Corresponding author: jjb12@cam.ac.uk
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Phys. Rev. Lett. 131, 126902 – Published 22 September, 2023

DOI: https://doi.org/10.1103/PhysRevLett.131.126902

Abstract

Strong coupling of molecular vibrations with light creates polariton states, enabling control over many optical and chemical properties. However, the near-field signatures of strong coupling are difficult to map as most cavities are closed systems. Surface-enhanced Raman microscopy of open metallic gratings under vibrational strong coupling enables the observation of spatial polariton localization in the grating near field, without the need for scanning probe microscopies. The lower polariton is localized at the grating slots, displays a strongly asymmetric line shape, and gives greater plasmon-vibration coupling strength than measured in the far field. Within these slots, the local field strength pushes the system into the ultrastrong coupling regime. Models of strong coupling which explicitly include the spatial distribution of emitters can account for these effects. Such gratings enable exploration of the rich physics of polaritons, its impact on polariton chemistry under flow conditions, and the interplay between near- and far-field properties through vibrational polariton-enhanced Raman scattering.

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synopsis

Metallic Gratings Produce a Strong Surprise

Published 22 September, 2023

Using a metallic grating and infrared light, researchers have uncovered a light–matter coupling regime where the local coupling strength can be 3.5 times higher than the global average for the material.

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Phys. Rev. Lett. 131, 126902– Published 22 September, 2023
  • Received 29 March 2023
  • Accepted 12 July 2023
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Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI.

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