Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

Mid-infrared radiative emission from bright hot plasmons in graphene

Abstract

Carrier excitation and decay processes in graphene are of broad interest since relaxation pathways that are not present in conventional materials are enabled by a gapless Dirac electronic band structure. Here, we report that a previously unobserved decay pathway—hot plasmon emission—results in Fermi-level-dependent mid-infrared emission in graphene. Our observations of non-thermal contributions to Fermi-level-dependent radiation are an experimental demonstration of hot plasmon emission arising from a photo-inverted carrier distribution in graphene achieved via ultrafast optical excitation. Our calculations indicate that the reported plasmon emission process can be several orders of magnitude brighter than Planckian emission mechanisms in the mid-infrared spectral range. Both the use of gold nanodisks to promote scattering and localized plasmon excitation and polarization-dependent excitation measurements provide further evidence for bright hot plasmon emission. These findings define an approach for future work on ultrafast and ultrabright graphene emission processes and mid-infrared light source applications.

Access options

Rent or Buy article

Get time limited or full article access on ReadCube.

from$8.99

All prices are NET prices.

Fig. 1: Carrier relaxation processes in graphene and experimental configuration.
Fig. 2: Fermi-level-dependent emission spectra in planar graphene.
Fig. 3: Non-equilibrium graphene plasmon dispersion and spontaneous plasmon emission spectra.
Fig. 4: Fermi-level-dependent emission spectra from graphene nanoribbon arrays.
Fig. 5: Enhancing radiation efficiency of bright hot plasmon emission with gold NDs on graphene.

Data availability

All measurement data are deposited in the Materials Cloud (https://doi.org/10.24435/materialscloud:sa-by), and other calculation data can be reproduced by the methods described in the Supplementary Information.

References

  1. 1.

    Jensen, S. A. et al. Competing ultrafast energy relaxation pathways in photoexcited graphene. Nano Lett. 14, 5839–5845 (2014).

    CAS  Article  Google Scholar 

  2. 2.

    Gierz, I. et al. Snapshots of non-equilibrium dirac carrier distributions in graphene. Nat. Mater. 12, 1119–1124 (2013).

    CAS  Article  Google Scholar 

  3. 3.

    Malard, L. M., Mak, K. F., Neto, A. H. C., Peres, N. M. R. & Heinz, T. F. Observation of intra- and inter-band transitions in the transient optical response of graphene. N. J. Phys. 15, 015009 (2013).

    CAS  Article  Google Scholar 

  4. 4.

    Sun, B. Y., Zhou, Y. & Wu, M. W. Dynamics of photoexcited carriers in graphene. Phys. Rev. B 85, 125413 (2012).

    Article  Google Scholar 

  5. 5.

    Breusing, M. et al. Ultrafast nonequilibrium carrier dynamics in a single graphene layer. Phys. Rev. B 83, 153410 (2011).

    Article  Google Scholar 

  6. 6.

    Tomadin, A. et al. The ultrafast dynamics and conductivity of photoexcited graphene at different Fermi energies. Sci. Adv. 4, eaar5313 (2018).

    Article  Google Scholar 

  7. 7.

    Kim, L. Novel Light Emitting Mechanisms Originating from Graphene Plasmons Near and Far from Equilibrium. PhD thesis, California Institute of Technology (2019).

  8. 8.

    Bostwick, A., Ohta, T., Seyller, T., Horn, K. & Rotenberg, E. Quasiparticle dynamics in graphene. Nat. Phys. 3, 36–40 (2007).

    CAS  Article  Google Scholar 

  9. 9.

    Polini, M. et al. Plasmons and the spectral function of graphene. Phys. Rev. B 77, 081411 (2008).

    Article  Google Scholar 

  10. 10.

    Hwang, E. H. & Das Sarma, S. Quasiparticle spectral function in doped graphene: electron-electron interaction effects in ARPES. Phys. Rev. B 77, 081412 (2008).

    Article  Google Scholar 

  11. 11.

    Hwang, E. H., Hu, B. Y. K. & Das Sarma, S. Inelastic carrier lifetime in graphene. Phys. Rev. B 76, 115434 (2007).

    Article  Google Scholar 

  12. 12.

    Rana, F. Graphene terahertz plasmon oscillators. IEEE Trans. Nanotechnol. 7, 91–99 (2008).

    Article  Google Scholar 

  13. 13.

    Rana, F., Strait, J. H., Wang, H. N. & Manolatou, C. Ultrafast carrier recombination and generation rates for plasmon emission and absorption in graphene. Phys. Rev. B. 84, 045437 (2011).

    Article  Google Scholar 

  14. 14.

    Hamm, J. M., Page, A. F., Bravo-Abad, J., Garcia-Vidal, F. J. & Hess, O. Nonequilibrium plasmon emission drives ultrafast carrier relaxation dynamics in photoexcited graphene. Phys. Rev. B 93, 041408 (2016).

    Article  Google Scholar 

  15. 15.

    Kim, S. et al. Electronically tunable extraordinary optical transmission in graphene plasmonic ribbons coupled to subwavelength metallic slit arrays. Nat. Commun. 7, 12323 (2016).

    CAS  Article  Google Scholar 

  16. 16.

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

    Article  Google Scholar 

  17. 17.

    Lui, C. H., Mak, K. F., Shan, J. & Heinz, T. F. Ultrafast photoluminescence from graphene. Phys. Rev. Lett. 105, 127404 (2010).

    Article  Google Scholar 

  18. 18.

    Alam, M. Z., De Leon, I. & Boyd, R. W. Large optical nonlinearity of indium tin oxide in its epsilon-near-zero region. Science 352, 795–797 (2016).

    CAS  Article  Google Scholar 

  19. 19.

    Huang, Y. W. et al. Gate-tunable conducting oxide metasurfaces. Nano Lett. 16, 5319–5325 (2016).

    CAS  Article  Google Scholar 

  20. 20.

    Page, A. F., Ballout, F., Hess, O. & Hamm, J. M. Nonequilibrium plasmons with gain in graphene. Phys. Rev. B 91, 075404 (2015).

    Article  Google Scholar 

  21. 21.

    Page, A. F., Hamm, J. M. & Hess, O. Polarization and plasmons in hot photoexcited graphene. Phys. Rev. B 97, 045428 (2018).

    CAS  Article  Google Scholar 

  22. 22.

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

    CAS  Article  Google Scholar 

  23. 23.

    Brar, V. W., Jang, M. S., Sherrott, M., Lopez, J. J. & Atwater, H. A. Highly confined tunable mid-infrared plasmonics in graphene nanoresonators. Nano Lett. 13, 2541–2547 (2013).

    CAS  Article  Google Scholar 

  24. 24.

    Han, S. et al. Complete complex amplitude modulation with electronically tunable graphene plasmonic metamolecules. ACS Nano 14, 1166–1175 (2020).

    CAS  Article  Google Scholar 

  25. 25.

    Kim, S., Menabde, S. G., Brar, V. W. & Jang, M. S. Functional mid-infrared polaritonics in van der Waals crystals. Adv. Opt. Mater. 8, 1901194 (2020).

  26. 26.

    Otsuji, T., Popov, V. & Ryzhii, V. Active graphene plasmonics for terahertz device applications. J. Phys. D 47, 094006 (2014).

    CAS  Article  Google Scholar 

  27. 27.

    Brar, V. W. et al. Electronic modulation of infrared radiation in graphene plasmonic resonators. Nat. Commun. 6, 7032 (2015).

    CAS  Article  Google Scholar 

  28. 28.

    Rana, F., George, P. A., Strait, J. H. & Dawlaty, J. Graphene terahertz sources and amplifiers. In Proc. 2008 33rd Int. Conf. on Infrared, Millimeter and Terahertz Waves 1–3 (IEEE, 2008).

  29. 29.

    Wagner, M. et al. Ultrafast and nanoscale plasmonic phenomena in exfoliated graphene revealed by infrared pump-probe nanoscopy. Nano Lett. 14, 894–900 (2014).

    CAS  Article  Google Scholar 

  30. 30.

    Ni, G. X. et al. Ultrafast optical switching of infrared plasmon polaritons in high-mobility graphene. Nat. Photon. 10, 244–247 (2016).

    CAS  Article  Google Scholar 

  31. 31.

    Zheng, B. Y. et al. Distinguishing between plasmon-induced and photoexcited carriers in a device geometry. Nat. Commun. 6, 7797 (2015).

    Article  Google Scholar 

  32. 32.

    Fang, Z. Y. et al. Plasmon-induced doping of graphene. ACS Nano 6, 10222–10228 (2012).

    CAS  Article  Google Scholar 

  33. 33.

    Song, S. M., Park, J. K., Sul, O. J. & Cho, B. J. Determination of work function of graphene under a metal electrode and its role in contact resistance. Nano Lett. 12, 3887–3892 (2012).

    CAS  Article  Google Scholar 

  34. 34.

    Boston Electronics LED55 and OPLED70 https://www.boselec.com (2021).

Download references

Acknowledgements

This work was supported by US Department of Energy Office of Science grant no. DE-FG02-07ER46405. V.W.B. was supported by a Defense Advanced Research Projects Agency Young Faculty Award (grant no. YFA D18AP00043) and by the Gordon and Betty Moore Foundation through a Moore Inventors Fellowship. S.K. acknowledges support by a Samsung Scholarship. Parts of the text and results reported in this work have been reproduced from the thesis by L. Kim, at the California Institute of Technology, and are accessible at https://thesis.library.caltech.edu/11500/.

Author information

Affiliations

Authors

Contributions

L.K., V.W.B. and H.A.A. conceived the ideas. L.K. performed spectroscopy experiments, and performed inversion and gain calculations as well as emissivity calculations. L.K. and S.K. fabricated the sample and performed data analysis. P.K.J. contributed to the discussion of the ratio of stimulated to spontaneous emission rates calculations. All authors cowrote the paper. V.W.B. and H.A.A. supervised the project.

Corresponding authors

Correspondence to Victor W. Brar or Harry A. Atwater.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Peer review information Nature Materials thanks Ortwin Hess, Frank Koppens and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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

Supplementary information

Supplementary Information

Supplementary Figs. 1–16 and Discussion.

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Kim, L., Kim, S., Jha, P.K. et al. Mid-infrared radiative emission from bright hot plasmons in graphene. Nat. Mater. (2021). https://doi.org/10.1038/s41563-021-00935-2

Download citation

Further reading

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing