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

Nature Photonics volume 15, pages 125–130 (2021)Cite this article

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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.

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Fig. 1: Wafer-scale resonant ENZ nanocavity platform for USC.
Fig. 2: Normal mode splittings due to ultrastrong plasmon–phonon coupling.
Fig. 3: Dispersion mapping and validation of theoretical model.

Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request.

References

  1. Törmä, P. & Barnes, W. L. Strong coupling between surface plasmon polaritons and emitters: a review. Rep. Prog. Phys. 78, 013901 (2015).

    ADS  Google Scholar 

  2. Ebbesen, T. W. Hybrid light-matter states in a molecular and material science perspective. Acc. Chem. Res. 49, 2403–2412 (2016).

    Google Scholar 

  3. Pelton, M. Modified spontaneous emission in nanophotonic structures. Nat. Photon. 9, 427–435 (2015).

    ADS  Google Scholar 

  4. Luk’yanchuk, B. et al. The Fano resonance in plasmonic nanostructures and metamaterials. Nat. Mater. 9, 707–715 (2010).

    ADS  Google Scholar 

  5. Neubrech, F. et al. Resonant plasmonic and vibrational coupling in a tailored nanoantenna for infrared detection. Phys. Rev. Lett. 101, 157403 (2008).

    ADS  Google Scholar 

  6. Yoshie, T. et al. Vacuum Rabi splitting with a single quantum dot in a photonic crystal nanocavity. Nature 432, 200–203 (2004).

    ADS  Google Scholar 

  7. Reithmaier, J. P. et al. Strong coupling in a single quantum dot-semiconductor microcavity system. Nature 432, 197–200 (2004).

    ADS  Google Scholar 

  8. Aoki, T. et al. Observation of strong coupling between one atom and a monolithic microresonator. Nature 443, 671–674 (2006).

    ADS  Google Scholar 

  9. Liu, X. et al. Strong light–matter coupling in two-dimensional atomic crystals. Nat. Photon. 9, 30–34 (2015).

    ADS  Google Scholar 

  10. Benz, F. et al. Single-molecule optomechanics in ‘picocavities’. Science 354, 726–729 (2016).

    ADS  Google Scholar 

  11. Santhosh, K., Bitton, O., Chuntonov, L. & Haran, G. Vacuum Rabi splitting in a plasmonic cavity at the single quantum emitter limit. Nat. Commun. 7, 11823 (2016).

    ADS  Google Scholar 

  12. Runnerstrom, E. L. et al. Polaritonic hybrid-epsilon-near-zero modes: beating the plasmonic confinement vs propagation-length trade-off with doped cadmium oxide bilayers. Nano Lett. 19, 948–957 (2018).

    ADS  Google Scholar 

  13. Leng, H., Szychowski, B., Daniel, M.-C. & Pelton, M. Strong coupling and induced transparency at room temperature with single quantum dots and gap plasmons. Nat. Commun. 9, 4012 (2018).

    ADS  Google Scholar 

  14. Park, K.-D. et al. Tip-enhanced strong coupling spectroscopy, imaging, and control of a single quantum emitter. Sci. Adv. 5, eaav5931 (2019).

    ADS  Google Scholar 

  15. Schoelkopf, R. J. & Girvin, S. M. Wiring up quantum systems. Nature 451, 664–669 (2008).

    ADS  Google Scholar 

  16. Dunkelberger, A., Spann, B., Fears, K., Simpkins, B. & Owrutsky, J. Modified relaxation dynamics and coherent energy exchange in coupled vibration-cavity polaritons. Nat. Commun. 7, 13504 (2016).

    ADS  Google Scholar 

  17. Munkhbat, B., Wersäll, M., Baranov, D. G., Antosiewicz, T. J. & Shegai, T. Suppression of photo-oxidation of organic chromophores by strong coupling to plasmonic nanoantennas. Sci. Adv. 4, eaas9552 (2018).

    ADS  Google Scholar 

  18. Thomas, A. et al. Tilting a ground-state reactivity landscape by vibrational strong coupling. Science 363, 615–619 (2019).

    ADS  Google Scholar 

  19. Kockum, A. F., Miranowicz, A., Liberato, S. D., Savasta, S. & Nori, F. Ultrastrong coupling between light and matter. Nat. Rev. Phys. 1, 19–40 (2019).

    Google Scholar 

  20. Forn-Díaz, P., Lamata, L., Rico, E., Kono, J. & Solano, E. Ultrastrong coupling regimes of light-matter interaction. Rev. Mod. Phys. 91, 025005 (2019).

    ADS  Google Scholar 

  21. Romero, G., Ballester, D., Wang, Y. M., Scarani, V. & Solano, E. Ultrafast quantum gates in circuit QED. Phys. Rev. Lett. 108, 120501 (2012).

    ADS  Google Scholar 

  22. Johansson, J. R., Johansson, G., Wilson, C. M. & Nori, F. Dynamical Casimir effect in a superconducting coplanar waveguide. Phys. Rev. Lett. 103, 147003 (2009).

    ADS  Google Scholar 

  23. Wilson, C. M. et al. Observation of the dynamical Casimir effect in a superconducting circuit. Nature 479, 376–379 (2011).

    ADS  Google Scholar 

  24. Schwartz, T., Hutchison, J. A., Genet, C. & Ebbesen, T. W. Reversible switching of ultrastrong light-molecule coupling. Phys. Rev. Lett. 106, 196405 (2011).

    ADS  Google Scholar 

  25. Niemczyk, T. et al. Circuit quantum electrodynamics in the ultrastrong-coupling regime. Nat. Phys. 6, 772–776 (2010).

    Google Scholar 

  26. Jouy, P. et al. Transition from strong to ultrastrong coupling regime in mid-infrared metal-dielectric-metal cavities. Appl. Phys. Lett. 98, 231114 (2011).

    ADS  Google Scholar 

  27. George, J. et al. Multiple Rabi splittings under ultrastrong vibrational coupling. Phys. Rev. Lett. 117, 153601 (2016).

    ADS  Google Scholar 

  28. Scalari, G. et al. Ultrastrong coupling of the cyclotron transition of a 2D electron gas to a THz metamaterial. Science 335, 1323–1326 (2012).

    ADS  Google Scholar 

  29. Shelton, D. J. et al. Strong coupling between nanoscale metamaterials and phonons. Nano Lett. 11, 2104–2108 (2011).

    ADS  Google Scholar 

  30. Autore, M. et al. Boron nitride nanoresonators for phonon-enhanced molecular vibrational spectroscopy at the strong coupling limit. Light Sci. Appl. 7, 17172 (2018).

    Google Scholar 

  31. Lather, J., Bhatt, P., Thomas, A., Ebbesen, T. W. & George, J. Cavity catalysis by cooperative vibrational strong coupling of reactant and solvent molecules. Angew. Chem. Int. Ed. 58, 10635–10638 (2019).

    Google Scholar 

  32. Jin, X. et al. Reshaping the phonon energy landscape of nanocrystals inside a terahertz plasmonic nanocavity. Nat. Commun. 9, 763 (2018).

    ADS  Google Scholar 

  33. Muller, E. A. et al. Nanoimaging and control of molecular vibrations through electromagnetically induced scattering reaching the strong coupling regime. ACS Photonics 5, 3594–3600 (2018).

    Google Scholar 

  34. Baida, F. I., Belkhir, A., Labeke, D. V. & Lamrous, O. Subwavelength metallic coaxial waveguides in the optical range: role of the plasmonic modes. Phys. Rev. B 74, 205419 (2006).

    ADS  Google Scholar 

  35. Alù, A. & Engheta, N. Light squeezing through arbitrarily shaped plasmonic channels and sharp bends. Phys. Rev. B 78, 035440 (2008).

    ADS  Google Scholar 

  36. Yoo, D. et al. High-throughput fabrication of resonant metamaterials with ultrasmall coaxial apertures via atomic layer lithography. Nano Lett. 16, 2040–2046 (2016).

    ADS  Google Scholar 

  37. Liberal, I. & Engheta, N. Near-zero refractive index photonics. Nat. Photon. 11, 149–158 (2017).

    ADS  MATH  Google Scholar 

  38. Lindquist, N. C., Nagpal, P., McPeak, K. M., Norris, D. J. & Oh, S.-H. Engineering metallic nanostructures for plasmonics and nanophotonics. Rep. Prog. Phys. 75, 036501 (2012).

    ADS  Google Scholar 

  39. Garcia-Vidal, F. J., Martin-Moreno, L., Ebbesen, T. W. & Kuipers, L. Light passing through subwavelength apertures. Rev. Mod. Phys. 82, 729–787 (2010).

    ADS  Google Scholar 

  40. Born, M. & Huang, K. Dynamical Theory of Crystal Lattices (Oxford Univ. Press, 1988).

  41. Hopfield, J. J. Theory of the contribution of excitons to the complex dielectric constant of crystals. Phys. Rev. 112, 1555–1567 (1958).

    ADS  MATH  Google Scholar 

  42. Quattropani, A., Andreani, L. C. & Bassani, F. Quantum theory of polaritons with spatial dispersion: exact solutions. Il Nuovo Cimento D 7, 55–69 (1986).

    ADS  Google Scholar 

  43. Ciuti, C., Bastard, G. & Carusotto, I. Quantum vacuum properties of the intersubband cavity polariton field. Phys. Rev. B 72, 115303 (2005).

    ADS  Google Scholar 

  44. Todorov, Y. & Sirtori, C. Intersubband polaritons in the electrical dipole gauge. Phys. Rev. B 85, 045304 (2012).

    ADS  Google Scholar 

  45. Kéna-Cohen, S., Maier, S. A. & Bradley, D. D. C. Ultrastrongly coupled exciton-polaritons in metal-clad organic semiconductor microcavities. Adv. Opt. Mater. 1, 827–833 (2013).

    Google Scholar 

  46. Cirio, M., De Liberato, S., Lambert, N. & Nori, F. Ground state electroluminescence. Phys. Rev. Lett. 116, 113601 (2016).

    ADS  Google Scholar 

  47. Kockum, A. F., Miranowicz, A., Macrì, V., Savasta, S. & Nori, F. Deterministic quantum nonlinear optics with single atoms and virtual photons. Phys. Rev. A 95, 063849 (2017).

    ADS  Google Scholar 

  48. Garziano, L. et al. One photon can simultaneously excite two or more atoms. Phys. Rev. Lett. 117, 043601 (2016).

    ADS  Google Scholar 

  49. Kockum, A. F., Macrì, V., Garziano, L., Savasta, S. & Nori, F. Frequency conversion in ultrastrong cavity QED. Sci. Rep. 7, 5313 (2017).

    ADS  Google Scholar 

  50. Kischkat, J. et al. Mid-infrared optical properties of thin films of aluminum oxide, titanium dioxide, silicon dioxide, aluminum nitride, and silicon nitride. Appl. Opt. 51, 6789–6898 (2012).

    ADS  Google Scholar 

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Acknowledgements

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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Author notes

  1. These authors contributed equally: Daehan Yoo, Fernando de León-Pérez.

Authors and Affiliations

  1. Department of Electrical and Computer Engineering, University of Minnesota, Minneapolis, MN, USA

    Daehan Yoo, In-Ho Lee, Daniel A. Mohr & Sang-Hyun Oh

  2. Centro Universitario de la Defensa de Zaragoza, Zaragoza, Spain

    Fernando de León-Pérez

  3. Instituto de Nanociencia y Materiales de Aragón (INMA) and Departamento de Física de la Materia Condensada, CSIC-Universidad de Zaragoza, Zaragoza, Spain

    Fernando de León-Pérez & Luis Martín-Moreno

  4. Department of Physics, University of Maryland, Baltimore County, Baltimore, MD, USA

    Matthew Pelton

  5. Department of Physics and JILA, University of Colorado, Boulder, CO, USA

    Markus B. Raschke

  6. Department of Mechanical Engineering, Vanderbilt University, Nashville, TN, USA

    Joshua D. Caldwell

Authors
  1. Daehan Yoo
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Contributions

D.Y. and S.-H.O. conceived the project and designed experiments. D.Y. performed device design, fabrication and measurements. F.d.L.-P. and L.M.-M. developed theories and performed numerical calculations. D.A.M. and I.-H.L. performed computer simulations. D.Y., F.d.L.-P., M.P., D.A.M., I.-H.L., M.B.R., J.D.C., L.M.-M. and S.-H.O. analysed the results. All authors contributed to interpretation of the results and wrote the paper together.

Corresponding authors

Correspondence to Luis Martín-Moreno or Sang-Hyun Oh.

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Supplementary Figs. 1–9, Sections 1–11 and Tables 1 and 2.

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Yoo, D., de León-Pérez, F., Pelton, M. et al. Ultrastrong plasmon–phonon coupling via epsilon-near-zero nanocavities. Nat. Photonics 15, 125–130 (2021). https://doi.org/10.1038/s41566-020-00731-5

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