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

Rakesh Arul; Kishan Menghrajani; Marie S. Rider; Rohit Chikkaraddy; William L.  Barnes; Jeremy J. Baumberg

doi:10.1103/PhysRevLett.131.126902

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

Rakesh Arul, Kishan Menghrajani, Marie S. Rider, Rohit Chikkaraddy, William L. Barnes^*, Jeremy J. Baumberg^*

^*Corresponding author for this work

Physics and Astronomy

Research output: Contribution to journal › Letter › peer-review

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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.

Original language	English
Article number	12902
Number of pages	6
Journal	Physical Review Letters
Volume	131
Issue number	12
DOIs	https://doi.org/10.1103/PhysRevLett.131.126902
Publication status	Published - 22 Sept 2023

Bibliographical note

Acknowledgments:
We acknowledge useful discussions with Rubén Esteban, Unai Muniain, and Javier Aizpurua. We acknowledge support from European Research Council (ERC) under Horizon 2020 research and innovation programme THOR (Grant Agreement No. 829067), PICOFORCE (Grant Agreement No. 883703), and project PHOTMAT (Grant Agreement ERC-2016-AdG-742222). R. A. acknowledges support from the Rutherford Foundation of the Royal Society Te Apãrangi of New Zealand, and the Winton Programme for the Physics of Sustainability. R. C. and R. A. acknowledge support from Trinity College, University of Cambridge. K. S. M. acknowledges financial support from the Leverhulme Trust research grant “Synthetic biological control of quantum optics”.

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title = "Raman Probing the Local Ultrastrong Coupling of Vibrational Plasmon Polaritons on Metallic Gratings",

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.",

author = "Rakesh Arul and Kishan Menghrajani and Rider, {Marie S.} and Rohit Chikkaraddy and Barnes, {William L.} and Baumberg, {Jeremy J.}",

note = "Acknowledgments: We acknowledge useful discussions with Rub{\'e}n Esteban, Unai Muniain, and Javier Aizpurua. We acknowledge support from European Research Council (ERC) under Horizon 2020 research and innovation programme THOR (Grant Agreement No. 829067), PICOFORCE (Grant Agreement No. 883703), and project PHOTMAT (Grant Agreement ERC-2016-AdG-742222). R. A. acknowledges support from the Rutherford Foundation of the Royal Society Te Ap{\~a}rangi of New Zealand, and the Winton Programme for the Physics of Sustainability. R. C. and R. A. acknowledge support from Trinity College, University of Cambridge. K. S. M. acknowledges financial support from the Leverhulme Trust research grant “Synthetic biological control of quantum optics”.",

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AU - Barnes, William L.

AU - Baumberg, Jeremy J.

N1 - Acknowledgments: We acknowledge useful discussions with Rubén Esteban, Unai Muniain, and Javier Aizpurua. We acknowledge support from European Research Council (ERC) under Horizon 2020 research and innovation programme THOR (Grant Agreement No. 829067), PICOFORCE (Grant Agreement No. 883703), and project PHOTMAT (Grant Agreement ERC-2016-AdG-742222). R. A. acknowledges support from the Rutherford Foundation of the Royal Society Te Apãrangi of New Zealand, and the Winton Programme for the Physics of Sustainability. R. C. and R. A. acknowledge support from Trinity College, University of Cambridge. K. S. M. acknowledges financial support from the Leverhulme Trust research grant “Synthetic biological control of quantum optics”.

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N2 - 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.

AB - 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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DO - 10.1103/PhysRevLett.131.126902

M3 - Letter

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JF - Physical Review Letters

IS - 12

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ER -

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

Abstract

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