Article | Published:

Graphene acoustic plasmon resonator for ultrasensitive infrared spectroscopy

Nature Nanotechnology (2019) | Download Citation


One of the fundamental hurdles in plasmonics is the trade-off between electromagnetic field confinement and the coupling efficiency with free-space light, a consequence of the large momentum mismatch between the excitation source and plasmonic modes. Acoustic plasmons in graphene, in particular, have an extreme level of field confinement, as well as an extreme momentum mismatch. Here, we show that this fundamental compromise can be overcome and demonstrate a graphene acoustic plasmon resonator with nearly perfect absorption (94%) of incident mid-infrared light. This high efficiency is achieved by utilizing a two-stage coupling scheme: free-space light coupled to conventional graphene plasmons, which then couple to ultraconfined acoustic plasmons. To realize this scheme, we transfer unpatterned large-area graphene onto template-stripped ultraflat metal ribbons. A monolithically integrated optical spacer and a reflector further boost the enhancement. We show that graphene acoustic plasmons allow ultrasensitive measurements of absorption bands and surface phonon modes in ångström-thick protein and SiO2 layers, respectively. Our acoustic plasmon resonator platform is scalable and can harness the ultimate level of light–matter interactions for potential applications including spectroscopy, sensing, metasurfaces and optoelectronics.

Access optionsAccess options

Rent or Buy article

Get time limited or full article access on ReadCube.


All prices are NET prices.

Data availability

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

Additional information

Publisher’s note: Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.


  1. 1.

    Hwang, E. & Sarma, S. D. Dielectric function, screening, and plasmons in two-dimensional graphene. Phys. Rev. B 75, 205418 (2007).

  2. 2.

    Jablan, M., Buljan, H. & Soljačić, M. Plasmonics in graphene at infrared frequencies. Phys. Rev. B 80, 245435 (2009).

  3. 3.

    Koppens, F. H., Chang, D. E. & García de Abajo, F. J. Graphene plasmonics: a platform for strong light–matter interactions. Nano Lett. 11, 3370–3377 (2011).

  4. 4.

    Yan, H. et al. Damping pathways of mid-infrared plasmons in graphene nanostructures. Nat. Photon. 7, 394–399 (2013).

  5. 5.

    Wunsch, B., Stauber, T., Sols, F. & Guinea, F. Dynamical polarization of graphene at finite doping. New J. Phys. 8, 318 (2006).

  6. 6.

    Liu, M. et al. Graphene-based broadband optical modulator. Nature 474, 64–67 (2011).

  7. 7.

    Sensale-Rodriguez, B. et al. Broadband graphene terahertz modulators enabled by intraband transitions. Nat. Commun. 3, 780 (2012).

  8. 8.

    Sun, Z., Martinez, A. & Wang, F. Optical modulators with 2D layered materials. Nat. Photon. 10, 227–238 (2016).

  9. 9.

    Fang, Z. et al. Graphene-antenna sandwich photodetector. Nano Lett. 12, 3808–3813 (2012).

  10. 10.

    Freitag, M. et al. Photocurrent in graphene harnessed by tunable intrinsic plasmons. Nat. Commun. 4, 1951 (2013).

  11. 11.

    Koppens, F. et al. Photodetectors based on graphene, other two-dimensional materials and hybrid systems. Nat. Nanotechnol. 9, 780–793 (2014).

  12. 12.

    Liu, C.-H., Chang, Y.-C., Norris, T. B. & Zhong, Z. Graphene photodetectors with ultra-broadband and high responsivity at room temperature. Nat. Nanotechnol. 9, 273–278 (2014).

  13. 13.

    Goossens, S. et al. Broadband image sensor array based on graphene–CMOS integration. Nat. Photon. 11, 366–371 (2017).

  14. 14.

    Fallahi, A. & Perruisseau-Carrier, J. Design of tunable biperiodic graphene metasurfaces. Phys. Rev. B 86, 195408 (2012).

  15. 15.

    Biswas, S. R. et al. Tunable graphene metasurface reflectarray for cloaking, illusion, and focusing. Phys. Rev. Appl. 9, 034021 (2018).

  16. 16.

    Ju, L. et al. Graphene plasmonics for tunable terahertz metamaterials. Nat. Nanotechnol. 6, 630–634 (2011).

  17. 17.

    Sherrott, M. C. et al. Experimental demonstration of >230° phase modulation in gate-tunable graphene–gold reconfigurable mid-infrared metasurfaces. Nano Lett. 17, 3027–3034 (2017).

  18. 18.

    Bao, Q. et al. Broadband graphene polarizer. Nat. Photon. 5, 411–415 (2011).

  19. 19.

    Tymchenko, M., Nikitin, A. Y. & Martín-Moreno, L. Faraday rotation due to excitation of magnetoplasmons in graphene microribbons. ACS Nano 7, 9780–9787 (2013).

  20. 20.

    Li, Y. et al. Graphene plasmon enhanced vibrational sensing of surface-adsorbed layers. Nano Lett. 14, 1573–1577 (2014).

  21. 21.

    Rodrigo, D. et al. Mid-infrared plasmonic biosensing with graphene. Science 349, 165–168 (2015).

  22. 22.

    Hu, H. et al. Far-field nanoscale infrared spectroscopy of vibrational fingerprints of molecules with graphene plasmons. Nat. Commun. 7, 12334 (2016).

  23. 23.

    Britnell, L. et al. Strong light–matter interactions in heterostructures of atomically thin films. Science 340, 1311–1314 (2013).

  24. 24.

    Chen, J. et al. Optical nano-imaging of gate-tunable graphene plasmons. Nature 487, 77–81 (2012).

  25. 25.

    Fei, Z. et al. Gate-tuning of graphene plasmons revealed by infrared nano-imaging. Nature 487, 82–85 (2012).

  26. 26.

    Woessner, A. et al. Highly confined low-loss plasmons in graphene–boron nitride heterostructures. Nat. Mater. 14, 421–425 (2015).

  27. 27.

    Hwang, E. & Sarma, S. D. Plasmon modes of spatially separated double-layer graphene. Phys. Rev. B 80, 205405 (2009).

  28. 28.

    Principi, A., Asgari, R. & Polini, M. Acoustic plasmons and composite hole–acoustic plasmon satellite bands in graphene on a metal gate. Solid State Commun. 151, 1627–1630 (2011).

  29. 29.

    Francescato, Y., Giannini, V. & Maier, S. A. Strongly confined gap plasmon modes in graphene sandwiches and graphene-on-silicon. New J. Phys. 15, 063020 (2013).

  30. 30.

    Alonso-González, P. et al. Acoustic terahertz graphene plasmons revealed by photocurrent nanoscopy. Nat. Nanotechnol. 12, 31–35 (2017).

  31. 31.

    Lundeberg, M. B. et al. Tuning quantum nonlocal effects in graphene plasmonics. Science 357, 187–191 (2017).

  32. 32.

    Chen, S. et al. Acoustic graphene plasmon nanoresonators for field-enhanced infrared molecular spectroscopy. ACS Photon. 4, 3089–3097 (2017).

  33. 33.

    Iranzo, D. A. et al. Probing the ultimate plasmon confinement limits with a van der Waals heterostructure. Science 360, 291–295 (2018).

  34. 34.

    Nikitin, A. Y., Low, T. & Martín-Moreno, L. Anomalous reflection phase of graphene plasmons and its influence on resonators. Phys. Rev. B 90, 041407 (2014).

  35. 35.

    Jang, M. S. et al. Tunable large resonant absorption in a midinfrared graphene Salisbury screen. Phys. Rev. B 90, 165409 (2014).

  36. 36.

    Kim, S. et al. Electronically tunable perfect absorption in graphene. Nano Lett. 18, 971–979 (2018).

  37. 37.

    Nagpal, P., Lindquist, N. C., Oh, S.-H. & Norris, D. J. Ultrasmooth patterned metals for plasmonics and metamaterials. Science 325, 594–597 (2009).

  38. 38.

    Lindquist, N. C., Johnson, T. W., Norris, D. J. & Oh, S.-H. Monolithic integration of continuously tunable plasmonic nanostructures. Nano Lett. 11, 3526–3530 (2011).

  39. 39.

    Lee, I.-H. et al. Anisotropic acoustic plasmons in black phosphorus. ACS Photon. 5, 2208–2016 (2017).

  40. 40.

    Yoo, D. et al. High-contrast infrared absorption spectroscopy via mass-produced coaxial zero-mode resonators with sub-10 nm gaps. Nano Lett. 18, 1930–1936 (2018).

  41. 41.

    Adato, R. et al. Ultra-sensitive vibrational spectroscopy of protein monolayers with plasmonic nanoantenna arrays. Proc. Natl Acad. Sci. USA 106, 19227–19232 (2009).

  42. 42.

    Olson, C. & Lynch, D. W. Longitudinal-optical-phonon–plasmon coupling in GaAs. Phys. Rev. 177, 1231 (1969).

  43. 43.

    Perlin, P. et al. Investigation of longitudinal-optical phonon–plasmon coupled modes in highly conducting bulk GaN. Appl. Phys. Lett. 67, 2524–2526 (1995).

  44. 44.

    Passler, N. C. et al. Strong coupling of epsilon-near-zero phonon polaritons in polar dielectric heterostructures. Nano Lett. 18, 4285–4292 (2018).

  45. 45.

    Low, T. et al. Polaritons in layered two-dimensional materials. Nat. Mater. 16, 182–194 (2017).

  46. 46.

    Wang, J., Hernandez, Y., Lotya, M., Coleman, J. N. & Blau, W. J. Broadband nonlinear optical response of graphene dispersions. Adv. Mater. 21, 2430–2435 (2009).

  47. 47.

    Wright, A., Xu, X., Cao, J. & Zhang, C. Strong nonlinear optical response of graphene in the terahertz regime. Appl. Phys. Lett. 95, 072101 (2009).

  48. 48.

    Lim, G.-K. et al. Giant broadband nonlinear optical absorption response in dispersed graphene single sheets. Nat. Photon. 5, 554–560 (2011).

  49. 49.

    Gullans, M., Chang, D., Koppens, F., de Abajo, F. G. & Lukin, M. D. Single-photon nonlinear optics with graphene plasmons. Phys. Rev. Lett. 111, 247401 (2013).

  50. 50.

    Lundeberg, M. B. et al. Thermoelectric detection and imaging of propagating graphene plasmons. Nat. Mater. 16, 204 (2017).

  51. 51.

    Freitag, M., Chiu, H.-Y., Steiner, M., Perebeinos, V. & Avouris, P. Thermal infrared emission from biased graphene. Nat. Nanotechnol. 5, 497–501 (2010).

  52. 52.

    Low, T. & Avouris, P. Graphene plasmonics for terahertz to mid-infrared applications. ACS Nano 8, 1086–1101 (2014).

  53. 53.

    Liang, X. et al. Toward clean and crackless transfer of graphene. ACS Nano 5, 9144–9153 (2011).

  54. 54.

    Gunes, F. et al. Layer-by-layer doping of few-layer graphene film. ACS Nano 4, 4595–4600 (2010).

  55. 55.

    D’Arsié, L. et al. Stable, efficient p-type doping of graphene by nitric acid. RSC Adv. 6, 113185–113192 (2016).

  56. 56.

    Nikitin, A. Y., Guinea, F., Garcia-Vidal, F. & Martin-Moreno, L. Fields radiated by a nanoemitter in a graphene sheet. Phys. Rev. B 84, 195446 (2011).

  57. 57.

    Ordal, M. A., Bell, R. J., Alexander, R. W., Long, L. L. & Querry, M. R. Optical properties of Au, Ni, and Pb at submillimeter wavelengths. Appl. Opt. 26, 744–752 (1987).

  58. 58.

    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, 6789–6798 (2012).

  59. 59.

    Liberman, V. et al. Rational design and optimization of plasmonic nanoarrays for surface enhanced infrared spectroscopy. Opt. Express 20, 11953–11967 (2012).

Download references


This research was supported primarily by the National Science Foundation (NSF) through an MRSEC grant (to I.-H.L., T.L. and S.-H.O.), ECCS 1809723 (to I.-H.L., S.-H.O. and T.L.) and ECCS 1610333 (to D.Y. and S.-H.O.). T.L. and S.-H.O. also acknowledge support from the Institute for Mathematics and its Applications (IMA) at the University of Minnesota. S.-H.O. further acknowledges support from the Sanford P. Bordeau Endowed Chair at the University of Minnesota. The authors thank S. Kim and M. Jo for sharing silk fibroin samples. Device fabrication was performed at the Minnesota Nanofabrication Center at the University of Minnesota, which receives partial support from the NSF through the National Nanotechnology Coordinated Infrastructure (NNCI). Electron microscopy measurements were performed at the Characterization Facility, which has received capital equipment from NSF MRSEC.

Author information


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

    • In-Ho Lee
    • , Daehan Yoo
    • , Tony Low
    •  & Sang-Hyun Oh
  2. IBM T. J. Watson Research Center, Yorktown Heights, New York, NY, USA

    • Phaedon Avouris


  1. Search for In-Ho Lee in:

  2. Search for Daehan Yoo in:

  3. Search for Phaedon Avouris in:

  4. Search for Tony Low in:

  5. Search for Sang-Hyun Oh in:


I.-H.L. and S.-H.O. conceived the idea. I.-H.L. performed simulations, device fabrication and characterization. D.Y. performed SEM and AFM characterization. I.-H.L., P.A., T.L. and S.-H.O. performed theoretical analysis. All authors analysed the data and wrote the paper together.

Competing interests

The authors declare no competing interests.

Corresponding author

Correspondence to Sang-Hyun Oh.

Supplementary information

  1. Supplementary Information

    Supplementary Figures 1–21

About this article

Publication history