Ultrastrong plasmon–phonon coupling via epsilon-near-zero nanocavities

Daehan Yoo; Fernando de León-Pérez; Matthew Pelton; In Ho Lee; Daniel A. Mohr; Markus B. Raschke; Joshua D. Caldwell; Luis Martín-Moreno; Sang Hyun Oh

doi:10.1038/s41566-020-00731-5

Ultrastrong plasmon–phonon coupling via epsilon-near-zero nanocavities

Daehan Yoo, Fernando de León-Pérez, Matthew Pelton, In Ho Lee, Daniel A. Mohr, Markus B. Raschke, Joshua D. Caldwell, Luis Martín-Moreno, Sang Hyun Oh

Electrical and Computer Engineering

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

52 Scopus citations

Abstract

Vibrational ultrastrong coupling, where the light–matter coupling strength is comparable to the vibrational frequency of molecules, presents new opportunities to probe the interactions between molecules and zero-point fluctuations, harness cavity-modified chemical reactions and develop novel devices in the mid-infrared spectral range. Here we use epsilon-near-zero nanocavities filled with a model polar medium (SiO₂) to demonstrate ultrastrong coupling between phonons and gap plasmons. We present classical and quantum-mechanical models to quantitatively describe the observed plasmon–phonon ultrastrong coupling phenomena and demonstrate a modal splitting of up to 50% of the resonant frequency (normalized coupling strength η > 0.25). Our wafer-scale nanocavity platform will enable a broad range of vibrational transitions to be harnessed for ultrastrong coupling applications.

Original language	English (US)
Pages (from-to)	125-130
Number of pages	6
Journal	Nature Photonics
Volume	15
Issue number	2
DOIs	https://doi.org/10.1038/s41566-020-00731-5
State	Published - Feb 2021

Bibliographical note

Funding Information:
We thank T. W. Ebbesen for helpful comments. This research was supported by grants from the US National Science Foundation (ECCS 1809240 to D.Y., D.A.M., S.-H.O.; ECCS 1809723 to I.-H.L., S.-H.O.) and the Samsung Global Research Outreach (GRO) Program (to S.-H.O.). F.d.L.-P. and L.M.-M. acknowledge financial support from the Spanish Ministry of Economy and Competitivity through projects MAT2017-88358-C3-1-R and MAT2017-88358-C3-2-R and the Aragón Government project Q-MAD. M.P. acknowledges support from the US National Science Foundation (NSF DMR-1905135). M.B.R. acknowledges funding from the US National Science Foundation (NSF CHE-1709822). J.D.C. was supported by the Office of Naval Research Grant N00014-18-12107. S.-H.O. further acknowledges support from the Sanford P. Bordeau Chair in Electrical Engineering at the University of Minnesota.

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© 2020, The Author(s), under exclusive licence to Springer Nature Limited.

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abstract = "Vibrational ultrastrong coupling, where the light–matter coupling strength is comparable to the vibrational frequency of molecules, presents new opportunities to probe the interactions between molecules and zero-point fluctuations, harness cavity-modified chemical reactions and develop novel devices in the mid-infrared spectral range. Here we use epsilon-near-zero nanocavities filled with a model polar medium (SiO2) to demonstrate ultrastrong coupling between phonons and gap plasmons. We present classical and quantum-mechanical models to quantitatively describe the observed plasmon–phonon ultrastrong coupling phenomena and demonstrate a modal splitting of up to 50% of the resonant frequency (normalized coupling strength η > 0.25). Our wafer-scale nanocavity platform will enable a broad range of vibrational transitions to be harnessed for ultrastrong coupling applications.",

author = "Daehan Yoo and {de Le{\'o}n-P{\'e}rez}, Fernando and Matthew Pelton and Lee, {In Ho} and Mohr, {Daniel A.} and Raschke, {Markus B.} and Caldwell, {Joshua D.} and Luis Mart{\'i}n-Moreno and Oh, {Sang Hyun}",

note = "Funding Information: We thank T. W. Ebbesen for helpful comments. This research was supported by grants from the US National Science Foundation (ECCS 1809240 to D.Y., D.A.M., S.-H.O.; ECCS 1809723 to I.-H.L., S.-H.O.) and the Samsung Global Research Outreach (GRO) Program (to S.-H.O.). F.d.L.-P. and L.M.-M. acknowledge financial support from the Spanish Ministry of Economy and Competitivity through projects MAT2017-88358-C3-1-R and MAT2017-88358-C3-2-R and the Arag{\'o}n Government project Q-MAD. M.P. acknowledges support from the US National Science Foundation (NSF DMR-1905135). M.B.R. acknowledges funding from the US National Science Foundation (NSF CHE-1709822). J.D.C. was supported by the Office of Naval Research Grant N00014-18-12107. S.-H.O. further acknowledges support from the Sanford P. Bordeau Chair in Electrical Engineering at the University of Minnesota. Publisher Copyright: {\textcopyright} 2020, The Author(s), under exclusive licence to Springer Nature Limited.",

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N2 - Vibrational ultrastrong coupling, where the light–matter coupling strength is comparable to the vibrational frequency of molecules, presents new opportunities to probe the interactions between molecules and zero-point fluctuations, harness cavity-modified chemical reactions and develop novel devices in the mid-infrared spectral range. Here we use epsilon-near-zero nanocavities filled with a model polar medium (SiO2) to demonstrate ultrastrong coupling between phonons and gap plasmons. We present classical and quantum-mechanical models to quantitatively describe the observed plasmon–phonon ultrastrong coupling phenomena and demonstrate a modal splitting of up to 50% of the resonant frequency (normalized coupling strength η > 0.25). Our wafer-scale nanocavity platform will enable a broad range of vibrational transitions to be harnessed for ultrastrong coupling applications.

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Ultrastrong plasmon–phonon coupling via epsilon-near-zero nanocavities

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