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Infrared nano-imaging of Dirac magnetoexcitons in graphene

Nature Nanotechnology volume 18, pages 1409–1415 (2023)Cite this article

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An Author Correction to this article was published on 17 November 2023

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Abstract

Magnetic fields can have profound effects on the motion of electrons in quantum materials. Two-dimensional electron systems subject to strong magnetic fields are expected to exhibit quantized Hall conductivity, chiral edge currents and distinctive collective modes referred to as magnetoplasmons and magnetoexcitons. Generating these propagating collective modes in charge-neutral samples and imaging them at their native nanometre length scales have thus far been experimentally elusive. Here we visualize propagating magnetoexciton polaritons at their native length scales and report their magnetic-field-tunable dispersion in near-charge-neutral graphene. Imaging these collective modes and their associated nano-electro-optical responses allows us to identify polariton-modulated optical and photo-thermal electric effects at the sample edges, which are the most pronounced near charge neutrality. Our work is enabled by innovations in cryogenic near-field optical microscopy techniques that allow for the nano-imaging of the near-field responses of two-dimensional materials under magnetic fields up to 7 T. This nano-magneto-optics approach allows us to explore and manipulate magnetopolaritons in specimens with low carrier doping via harnessing high magnetic fields.

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Fig. 1: Magnetic field-dependent m-SNOM and near-field photocurrent DiME measurements of hBN-encapsulated graphene at 200 K.
Fig. 2: Nano-infrared images of near-charge-neutral graphene in the regime of the field-tuned 0 → 1 LL transition.
Fig. 3: Magnetic field tuning of DiMEs.
Fig. 4: Magnetic field-dependent DiMEs dispersion.

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Data availability

The data represented in Figs. 1–4 are available as Source Data 1–4. All other data that support the findings of this study are available from the corresponding authors upon reasonable request.

Code availability

All codes underlying this study are available from the corresponding authors upon reasonable request.

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References

  1. Peres, N. M. R., Guinea, F. & Castro Neto, A. H. Electronic properties of disordered two-dimensional carbon. Phys. Rev. B Condens. Matter Mater. Phys. 73, 125411 (2006).

    Google Scholar 

  2. Sadowski, M. L., Martinez, G., Potemski, M., Berger, C. & De Heer, W. A. Landau level spectroscopy of ultrathin graphite layers. Phys. Rev. Lett. 97, 266405 (2006).

    CAS  Google Scholar 

  3. Jiang, Z. et al. Infrared spectroscopy of Landau levels of graphene. Phys. Rev. Lett. 98, 197403 (2007).

    CAS  Google Scholar 

  4. Gusynin, V. P., Sharapov, S. G. & Carbotte, J. P. Magneto-optical conductivity in graphene. J. Phys. Condens. Matter 19, 026222 (2007).

    Google Scholar 

  5. Crassee, I. et al. Giant Faraday rotation in single- and multilayer graphene. Nat. Phys. 7, 48–51 (2011).

    CAS  Google Scholar 

  6. Crassee, I. et al. Multicomponent magneto-optical conductivity of multilayer graphene on SiC. Phys. Rev. B Condens. Matter Mater. Phys. 84, 035103 (2011).

    Google Scholar 

  7. Goerbig, M. O. Electronic properties of graphene in a strong magnetic field. Rev. Mod. Phys. 83, 1193 (2011).

    CAS  Google Scholar 

  8. Orlita, M. et al. Approaching the Dirac point in high-mobility multilayer epitaxial graphene. Phys. Rev. Lett. 101, 267601 (2008).

    CAS  Google Scholar 

  9. Kallin, C. & Halperin, B. I. Excitations from a filled Landau level in the two-dimensional electron gas. Phys. Rev. B 30, 5655 (1984).

    Google Scholar 

  10. Lozovik, Y. E. & Sokolik, A. A. Influence of Landau level mixing on the properties of elementary excitations in graphene in strong magnetic field. Nanoscale Res. Lett. 7, 134 (2012).

    Google Scholar 

  11. Wang, W., Apell, S. P. & Kinaret, J. M. Edge magnetoplasmons and the optical excitations in graphene disks. Phys. Rev. B Condens. Matter Mater. Phys. 86, 125450 (2012).

    Google Scholar 

  12. Andreev, I. V., Muravev, V. M., Semenov, N. D., Zabolotnykh, A. A. & Kukushkin, I. V. Magnetodispersion of two-dimensional plasmon polaritons. Phys. Rev. B 104, 195436 (2021).

    CAS  Google Scholar 

  13. Petković, I., Williams, F. I. B. & Glattli, D. C. Edge magnetoplasmons in graphene. J. Phys. D: Appl. Phys. 47, 094010 (2014).

    Google Scholar 

  14. Poumirol, J. M. et al. Electrically controlled terahertz magneto-optical phenomena in continuous and patterned graphene. Nat. Commun. 8, 14626 (2017).

    Google Scholar 

  15. Slipchenko, T. M., Poumirol, J. M., Kuzmenko, A. B., Nikitin, A. Y. & Martín-Moreno, L. Interband plasmon polaritons in magnetized charge-neutral graphene. Commun. Phys. 4, 110 (2021).

    CAS  Google Scholar 

  16. Iyengar, A., Wang, J., Fertig, H. A. & Brey, L. Excitations from filled Landau levels in graphene. Phys. Rev. B Condens. Matter Mater. Phys. 75, 125430 (2007).

    Google Scholar 

  17. Keilmann, F. & Hillenbrand, R. Near-field microscopy by elastic light scattering from a tip. Phil. Trans. R. Soc. A 362, 787–805 (2004).

    CAS  Google Scholar 

  18. Chen, X. et al. Modern scattering-type scanning near-field optical microscopy for advanced material research. Adv. Mater. 31, 1804774 (2019).

    Google Scholar 

  19. Dapolito, M. et al. Scattering-type scanning near-field optical microscopy with Akiyama piezo-probes. Appl. Phys. Lett. 120, 013104 (2022).

    CAS  Google Scholar 

  20. Fei, Z. et al. Edge and surface plasmons in graphene nanoribbons. Nano Lett. 15, 8271–8276 (2015).

    CAS  Google Scholar 

  21. Sunku, S. S. et al. Photonic crystals for nano-light in moiré graphene superlattices. Science 362, 1153–1156 (2018).

    CAS  Google Scholar 

  22. Lundeberg, M. B. et al. Thermoelectric detection and imaging of propagating graphene plasmons. Nat. Mater. 16, 204–207 (2017).

    CAS  Google Scholar 

  23. Jing, R. et al. Terahertz response of monolayer and few-layer WTe2 at the nanoscale. Nat. Commun. 12, 5594 (2021).

    CAS  Google Scholar 

  24. Qazilbash, M. M. et al. Mott transition in VO2 revealed by infrared spectroscopy and nano-imaging. Science 318, 1750–1753 (2007).

    CAS  Google Scholar 

  25. McLeod, A. S. et al. Nanotextured phase coexistence in the correlated insulator V2O3. Nat. Phys. 13, 80–86 (2017).

    CAS  Google Scholar 

  26. Post, K. W. et al. Coexisting first- and second-order electronic phase transitions in a correlated oxide. Nat. Phys. 14, 1056–1061 (2018).

    CAS  Google Scholar 

  27. Stinson, H. T. et al. Imaging the nanoscale phase separation in vanadium dioxide thin films at terahertz frequencies. Nat. Commun. 9, 3604 (2018).

    CAS  Google Scholar 

  28. Sunku, S. S. et al. Nano-photocurrent mapping of local electronic structure in twisted bilayer graphene. Nano Lett. 20, 2958–2964 (2020).

    CAS  Google Scholar 

  29. Woessner, A. et al. Near-field photocurrent nanoscopy on bare and encapsulated graphene. Nat. Commun. 7, 10783 (2016).

    CAS  Google Scholar 

  30. Shao, Y. et al. Nonlinear nanoelectrodynamics of a Weyl metal. Proc. Natl Acad. Sci. USA 118, e2116366118 (2021).

    CAS  Google Scholar 

  31. Sunku, S. S. et al. Hyperbolic enhancement of photocurrent patterns in minimally twisted bilayer graphene. Nat. Commun. 12, 1641 (2021).

    CAS  Google Scholar 

  32. Nedoliuk, I. O., Hu, S., Geim, A. K. & Kuzmenko, A. B. Colossal infrared and terahertz magneto-optical activity in a two-dimensional Dirac material. Nat. Nanotechnol. 14, 756–761 (2019).

    CAS  Google Scholar 

  33. Kotov, V. N., Uchoa, B., Pereira, V. M., Guinea, F. & Castri Neto, A. H. Electron-electron interactions in graphene: current status and perspectives. Rev. Mod. Phys. 84, 1067 (2012).

    CAS  Google Scholar 

  34. Shizuya, K. Many-body corrections to cyclotron resonance in monolayer and bilayer graphene. Phys. Rev. B 81, 075407 (2010).

    Google Scholar 

  35. Henriksen, E. A. et al. Interaction-induced shift of the cyclotron resonance of graphene using infrared spectroscopy. Phys. Rev. Lett. 104, 067404 (2010).

    CAS  Google Scholar 

  36. Xu, X., Gabor, N. M., Alden, J. S., Van Der Zande, A. M. & McEuen, P. L. Photo-thermoelectric effect at a graphene interface junction. Nano Lett. 10, 562–566 (2010).

    CAS  Google Scholar 

  37. Checkelsky, J. G. & Ong, N. P. Thermopower and Nernst effect in graphene in a magnetic field. Phys. Rev. B 80, 081413(R) (2009).

    Google Scholar 

  38. Wei, P., Bao, W., Pu, Y., Lau, C. N. & Shi, J. Anomalous thermoelectric transport of Dirac particles in graphene. Phys. Rev. Lett. 102, 166808 (2009).

    Google Scholar 

  39. Lundeberg, M. B. & Koppens, F. H. L. Thermodynamic reciprocity in scanning photocurrent maps. Preprint at https://arxiv.org/abs/2011.04311 (2020).

  40. Cao, H. et al. Photo-Nernst current in graphene. Nat. Phys. 12, 236–239 (2016).

    CAS  Google Scholar 

  41. Olbrich, P. et al. Giant photocurrents in a Dirac fermion system at cyclotron resonance. Phys. Rev. B Condens. Matter Mater. Phys. 87, 235439 (2013).

    Google Scholar 

  42. Fei, Z. et al. Gate-tuning of graphene plasmons revealed by infrared nano-imaging. Nature 486, 82–85 (2012).

    Google Scholar 

  43. Alonso-González, P. et al. Acoustic terahertz graphene plasmons revealed by photocurrent nanoscopy. Nat. Nanotechnol. 12, 31–35 (2016).

    Google Scholar 

  44. Giubileo, F. & Di Bartolomeo, A. The role of contact resistance in graphene field-effect devices. Prog. Surf. Sci. 92, 143–175 (2017).

    CAS  Google Scholar 

  45. Chen, X. et al. Rapid simulations of hyperspectral near-field images of three-dimensional heterogeneous surfaces—part II. Opt. Express 30, 11228 (2022).

    CAS  Google Scholar 

  46. Maissen, C., Chen, S., Nikulina, E., Govyadinov, A. & Hillenbrand, R. Probes for ultrasensitive THz nanoscopy. ACS Photonics 6, 1279–1288 (2019).

    CAS  Google Scholar 

  47. Xin, N. et al. Giant magnetoresistance of Dirac plasma in high-mobility graphene. Nature 616, 270–274 (2023).

    CAS  Google Scholar 

  48. Li, Q. et al. Chiral magnetic effect in ZrTe5. Nat. Phys. 12, 550–554 (2016).

    Google Scholar 

  49. Tseng, C. C. et al. Gate-tunable proximity effects in graphene on layered magnetic insulators. Nano Lett. 22, 8495–8501 (2022).

    CAS  Google Scholar 

  50. Bloch, J., Cavalleri, A., Galitski, V., Hafezi, M. & Rubio, A. Strongly correlated electron–photon systems. Nature 606, 41–48 (2022).

    CAS  Google Scholar 

  51. Ma, C. et al. Moiré band topology in twisted bilayer graphene. Nano Lett. 20, 6076–6083 (2020).

    CAS  Google Scholar 

  52. Yu, J. et al. Correlated Hofstadter spectrum and flavour phase diagram in magic-angle twisted bilayer graphene. Nat. Phys. 18, 825–831 (2022).

    CAS  Google Scholar 

  53. Hu, B., Tao, J., Zhang, Y. & Wang, Q. J. Magneto-plasmonics in graphene-dielectric sandwich. Opt. Express 22, 21727 (2014).

    Google Scholar 

  54. Yan, H. et al. Infrared spectroscopy of tunable Dirac terahertz magneto-plasmons in graphene. Nano Lett. 12, 3766–3771 (2012).

    CAS  Google Scholar 

  55. Kim, R. H. J., Park, J.-M., Haeuser, S. J., Luo, L. & Wang, J. A sub-2 Kelvin cryogenic magneto-terahertz scattering-type scanning near-field optical microscope (cm-THz-sSNOM). Rev. Sci. Instrum. 94, 043702 (2023).

    CAS  Google Scholar 

  56. Fei, Z. et al. Infrared nanoscopy of Dirac plasmons at the graphene-SiO2 interface. Nano Lett. 11, 4701–4705 (2011).

    CAS  Google Scholar 

  57. Knoll, B. & Keilmann, F. Enhanced dielectric contrast in scattering-type scanning near-field optical microscopy. Opt. Commun. 182, 321–328 (2000).

    CAS  Google Scholar 

  58. Purdie, D. G. et al. Cleaning interfaces in layered materials heterostructures. Nat. Commun. 9, 5387 (2018).

    CAS  Google Scholar 

  59. Wang, L. et al. One-dimensional electrical contact to a two-dimensional material. Science 342, 614–617 (2013).

    CAS  Google Scholar 

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Acknowledgements

M.D., M.K.L. and Q.L. acknowledge support from the DOE, Office of Science, Basic Energy Sciences, Division of Materials Sciences and Engineering (Contract No. DE-SC0012704) for the construction of infrared optics and sample characterization. X.C., M.K.L and D.N.B. acknowledge the support of m-SNOM scanner construction as part of Programmable Quantum Materials, an Energy Frontier Research Center funded by the DOE, Office of Science, Basic Energy Sciences (Award DE-SC0019443). M.D., L.W., G.L.C, X.C, D.N.B. and M.K.L. acknowledge support of the Akiyama probe design from the US Department of Energy (DOE), Office of Science, National Quantum Information Science Research Centers, Co-design Center for Quantum Advantage (Contract No. DE-SC0012704). X.D. acknowledges support from the National Science Foundation (Award DMR-1808491). A.B.K. and A.B. are supported by the Swiss National Science Foundation (Grant No. 200020_201096). We are grateful for the helpful discussion and technical support from X. Xu at Lehigh University, D. Martien from Quantum Design, J. Li and W. Wang from Ithatron Optics, X. Wu from the Institute of Physics, Chinese Academy of Sciences, Q. Yang from Jilin University and Q. Sun from Tsinghua University.

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Authors and Affiliations

  1. Department of Physics and Astronomy, Stony Brook University, Stony Brook, NY, USA

    Michael Dapolito, Makoto Tsuneto, Wenjun Zheng, Lukas Wehmeier, Xinzhong Chen, Jiacheng Sun, Zengyi Du, Vibhu Ravindran, Zijian Zhou, Mila Petrovic, Qiang Li, Xu Du & Mengkun Liu

  2. Department of Physics, Columbia University, New York, NY, USA

    Michael Dapolito, Suheng Xu, Xinzhong Chen, Yinming Shao, Ran Jing, Shuai Zhang, Yinan Dong, Dorri Halbertal & D. N. Basov

  3. National Synchrotron Light Source II, Brookhaven National Laboratory, Upton, NY, USA

    Lukas Wehmeier, G. L. Carr & Mengkun Liu

  4. Département de Physique de la Matière Quantique, Université de Genève, Genève 4, Switzerland

    Adrien Bercher & Alexey B. Kuzmenko

  5. Department of Physics, University of California, Berkeley, CA, USA

    Vibhu Ravindran

  6. Department of Physics, Yale University, New Haven, CT, USA

    Adrian Gozar

  7. Energy Sciences Institute, Yale University, West Haven, CT, USA

    Adrian Gozar

  8. Condensed Matter Physics and Materials Science Division, Brookhaven National Laboratory, Upton, NY, USA

    Qiang Li

  9. Department of Physics, University of California at San Diego, La Jolla, CA, USA

    Michael M. Fogler

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  1. Michael Dapolito
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Contributions

M.D., M.T., X.C., L.W., W.Z., D.N.B. and M.K.L. designed the experiment. M.D., M.T., L.W., S.Z., X.D. and M.K.L. performed the measurements. X.D. and J.S. fabricated the samples. M.D., M.T., Z.D., X.C., L.W., W.Z. S.X., Y.D., V.R., M.P., Z.Z., A.B., G.L.C., Q.L., A.B.K., A.G., X.D., M.M.F. and M.K.L. analysed the data. M.T., X.C., W.Z., S.X., Y.S., R.J. and D.H. performed the simulations. M.D. and M.K.L wrote the paper. All authors contributed to the scientific discussions and paper revisions.

Corresponding authors

Correspondence to D. N. Basov, Xu Du or Mengkun Liu.

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Competing interests

M.D., X.C., M.K.L. and A.G. have a patent pending related to the design of the m-SNOM. The other authors declare no competing interests.

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Extended data

Extended Data Fig. 1 Closed-cycle m-SNOM setup.

OAP: off-axis parabolic mirror. Tip: Akiyama probe. Light enters the chamber in the horizontal direction (into the field of view) and is focused onto the sample with an OAP.

Supplementary information

Supplementary Information

Supplementary Notes 1–3 and Figs. 1–8.

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Source data

Source Data Fig. 1

Source data for Fig. 1d–f.

Source Data Fig. 2

Source data for Fig. 2a,b.

Source Data Fig. 3

Source data for Fig. 3b–d.

Source Data Fig. 4

Source data for Fig. 4a–d.

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Dapolito, M., Tsuneto, M., Zheng, W. et al. Infrared nano-imaging of Dirac magnetoexcitons in graphene. Nat. Nanotechnol. 18, 1409–1415 (2023). https://doi.org/10.1038/s41565-023-01488-y

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