Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Open Access

Ultrafast terahertz photoconductivity and near-field imaging of nanoscale inhomogeneities in multilayer epitaxial graphene nanoribbons

Arvind Singh1, Jan Kunc2, Tinkara Troha1, Hynek Němec1, and Petr Kužel1,*

  • *Contact author: kuzelp@fzu.cz

Phys. Rev. B 113, 115417 – Published 17 March, 2026

DOI: https://doi.org/10.1103/qzns-hs4t

Abstract

We study broadband terahertz (THz) conductivity and ultrafast photoconductivity spectra in lithographically fabricated multilayer epitaxial graphene nanoribbons grown on C-face of 6H-SiC substrate. THz near-field spectroscopy reveals local conductivity variations across nanoscale structural inhomogeneities such as wrinkles and grain boundaries within the multilayer graphene. Ultrabroadband THz far-field spectroscopy (0.15–16THz) distinguishes doped graphene layers near the substrate from quasineutral layers (QNLs) further from the substrate. Temperature-dependent THz conductivity spectra are dominated by intraband transitions both in the doped and QNLs. Photoexcitation then alters mainly the response of the QNLs: these exhibit very high carrier mobility and large positive THz photoconductivity with picosecond lifetime. The response of QNLs strongly depends on the carrier temperature Tc: the scattering time drops by an order of magnitude down to ∼10 fs upon an increase of Tc from 50 K to Tc>1000K, which is attributed to an enhanced electron-electron and electron-phonon scattering and to an interaction of electrons with mid-gap states.

View figure in article

Physics Subject Headings (PhySH)

Article Text

References (61)

  1. C. Berger, et al., Ultrathin epitaxial graphite: 2D electron gas properties and a route toward graphene-based nanoelectronics, J. Phys. Chem. B 108, 19912 (2004).
  2. C. Virojanadara, M. Syväjarvi, R. Yakimova, L. I. Johansson, A. A. Zakharov, and T. Balasubramanian, Homogeneous large-area graphene layer growth on 6H-SiC(0001), Phys. Rev. B 78, 245403 (2008).
  3. K. V. Emtsev, et al., Towards wafer-size graphene layers by atmospheric pressure graphitization of silicon carbide, Nat. Mater. 8, 203 (2009).
  4. Y.-M. Lin, C. Dimitrakopoulos, K. A. Jenkins, D. B. Farmer, H.-Y. Chiu, A. Grill, and Ph. Avouris, 100-GHz transistors from wafer-scale epitaxial graphene, Science 327, 662 (2010).
  5. J. Hass, F. Varchon, J. E. Millán-Otoya, M. Sprinkle, N. Sharma, W. A. de Heer, C. Berger, P. N. First, L. Magaud, and E. H. Conrad, Why multilayer graphene on 4H-SiC behaves like a single sheet of graphene, Phys. Rev. Lett. 100, 125504 (2008).
  6. J. Hass, R. Feng, J. E. Millán-Otoya, X. Li, M. Sprinkle, P. N. First, W. A. de Heer, E. H. Conrad, and C. Berger, Structural properties of the multilayer graphene/4H-SiC system as determined by surface x-ray diffraction, Phys. Rev. B 75, 214109 (2007).
  7. I. Crassee, J. Levallois, D. van der Marel, A. L. Walter, Th. Seyller, and A. B. Kuzmenko, Multicomponent magneto-optical conductivity of multilayer graphene on SiC, Phys. Rev. B 84, 035103 (2011).
  8. M. L. Sadowski, G. Martinez, M. Potemski, C. Berger, and W. A. de Heer, Landau level spectroscopy of ultrathin graphite layers, Phys. Rev. Lett. 97, 266405 (2006).
  9. M. Sprinkle, et al., First Direct observation of a nearly ideal graphene band structure, Phys. Rev. Lett. 103, 226803 (2009).
  10. D. Sun, C. Divin, C. Berger, W. A. de Heer, P. N. First, and T. B. Norris, Spectroscopic measurement of interlayer screening in multilayer epitaxial graphene, Phys. Rev. Lett. 104, 136802 (2010).
  11. J.-H. Chen, C. Jang, S. Xiao, M. Ishigami, and M. S. Fuhrer, Intrinsic and extrinsic performance limits of graphene devices on SiO2, Nat. Nanotechnol. 3, 206 (2008).
  12. E. H. Hwang and S. Das Sarma, Acoustic phonon scattering limited carrier mobility in two-dimensional extrinsic graphene, Phys. Rev. B 77, 115449 (2008).
  13. J. L. Tedesco, B. L. VanMil, R. L. Myers-Ward, J. M. McCrate, S. A. Kitt, P. M. Campbell, G. G. Jernigan, J. C. Culbertson, C. R. Eddy, Jr., and D. K. Gaskill, Hall effect mobility of epitaxial graphene grown on silicon carbide, Appl. Phys. Lett. 95, 122102 (2009).
  14. F. Speck, J. Jobst, F. Fromm, M. Ostler, D. Waldmann, M. Hundhausen, H. B. Weber, and Th. Seyller, The quasifree-standing nature of graphene on H-saturated SiC(0001), Appl. Phys. Lett. 99, 122106 (2011).
  15. V. C. Paingad, J. Kunc, M. Rejhon, I. Rychetský, I. Mohelský, M. Orlita, and P. Kužel, Ultrafast plasmon thermalization in epitaxial graphene probed by time-resolved THz spectroscopy, Adv. Funct. Mater. 31, 2105763 (2021).
  16. Y.-M. Lin, et al., Multicarrier transport in epitaxial multilayer graphene, Appl. Phys. Lett. 97, 112107 (2010).
  17. W. A. de Heer, et al., Epitaxial graphene, Solid State Commun. 143, 92 (2007).
  18. B. L. VanMil, R. L. Myers-Ward, J. L. Tedesco, C. R. Eddy, G. G. Jernigan, J. C. Culbertson, P. M. Campbell, J. M. McCrate, S. A. Kitt, and D. K. Gaskill, Graphene Formation on SiC Substrates, Mater. Sci. Forum 615–617, 211 (2009).
  19. M. Mittendorff, et al., Carrier dynamics in Landau-quantized graphene featuring strong Auger scattering, Nat. Phys. 11, 75 (2015).
  20. G. Li, V. Semenenko, V. Perebeinos, and P. Q. Liu, Multilayer graphene terahertz plasmonic structures for enhanced frequency tuning range, ACS Photonics 6, 3180 (2019).
  21. K. M. Daniels, M. M. Jadidi, A. B. Sushkov, A. Nath, A. K. Boyd, K. Sridhara, H. D. Drew, T. E. Murphy, R. L. Myers-Ward, and D. K. Gaskill, Narrow plasmon resonances enabled by quasifreestanding bilayer epitaxial graphene, 2D Mater. 4, 025034 (2017).
  22. J. W. Han, et al., Plasmonic terahertz nonlinearity in graphene disks, Adv. Photon. Res. 3, 2100218 (2022).
  23. S. D. Sarma, S. Adam, E. H. Hwang, and E. Rossi, Electronic transport in two-dimensional graphene, Rev. Mod. Phys. 83, 407 (2011).
  24. K. J. Tielrooij, J. C. W. Song, S. A. Jensen, A. Centeno, A. Pesquera, A. Zurutuza Elorza, M. Bonn, L. S. Levitov, and F. H. L. Koppens, Photoexcitation cascade and multiple hot-carrier generation in graphene, Nat. Phys. 9, 248 (2013).
  25. P. Kužel and H. Němec, Terahertz spectroscopy of nanomaterials: A close look at charge-carrier transport, Adv. Opt. Mater. 8, 1900623 (2020).
  26. M. M. Jadidi, K. M. Daniels, R. L. Myers-Ward, D. K. Gaskill, J. C. König-Otto, S. Winnerl, A. B. Sushkov, H. D. Drew, T. E. Murphy, and M. Mittendorff, Optical control of plasmonic hot carriers in graphene, ACS Photonics 6, 302 (2019).
  27. A. Tomadin, et al., The ultrafast dynamics and conductivity of photoexcited graphene at different Fermi energies, Sci. Adv. 4, eaar5313 (2018).
  28. M. Massicotte, G. Soavi, A. Principi, and K.-J. Tielrooij, Hot carriers in graphene – fundamentals and applications, Nanoscale 13, 8376 (2021).
  29. S. Kumar, M. Anija, N. Kamaraju, K. S. Vasu, K. S. Subrahmanyam, A. K. Sood, and C. N. R. Rao, Femtosecond carrier dynamics and saturable absorption in graphene suspensions, Appl. Phys. Lett. 95, 191911 (2009).
  30. A. Singh and S. Kumar, Terahertz photonics and optoelectronics of carbon-based nanosystems, J. Appl. Phys. 131, 160901 (2022).
  31. A. Singh and S. Kumar, Phonon bottleneck in temperature-dependent hot carrier relaxation in graphene oxide, J. Phys. Chem. C 125, 26583 (2021).
  32. A. Singh, H. Němec, J. Kunc, and P. Kužel, Ultrafast terahertz conductivity in epitaxial graphene nanoribbons: An interplay between photoexcited and secondary hot carriers, J. Phys. D Appl. Phys. 58, 045307 (2025).
  33. J. Nilsson, A. H. Castro Neto, F. Guinea, and N. M. R. Peres, Electronic properties of bilayer and multilayer graphene, Phys. Rev. B 78, 045405 (2008).
  34. M. Koshino and T. Ando, Magneto-optical properties of multilayer graphene, Phys. Rev. B 77, 115313 (2008).
  35. M. Orlita, et al., Approaching the Dirac point in high-mobility multilayer epitaxial graphene, Phys. Rev. Lett. 101, 267601 (2008).
  36. H. Choi, F. Borondics, D. A. Siegel, S. Y. Zhou, M. C. Martin, A. Lanzara, and R. A. Kaindl, Broadband electromagnetic response and ultrafast dynamics of few-layer epitaxial graphene, Appl. Phys. Lett. 94, 172102 (2009).
  37. M. T. Mihnev, J. R. Tolsma, C. J. Divin, D. Sun, R. Asgari, M. Polini, C. Berger, W. A. de Heer, A. H. MacDonald, and T. B. Norris, Electronic cooling via interlayer Coulomb coupling in multilayer epitaxial graphene, Nat. Commun. 6, 8105 (2015).
  38. S. Massabeau, M. Baillergeau, T. Phuphachong, C. Berger, W. A. de Heer, S. Dhillon, J. Tignon, L. A. de Vaulchier, R. Ferreira, and J. Mangeney, Evidence of Fermi level pinning at the Dirac point in epitaxial multilayer graphene, Phys. Rev. B 95, 085311 (2017).
  39. C. Berger, et al., Electronic confinement and coherence in patterned epitaxial graphene, Science 312, 1191 (2006).
  40. M. L. Sadowski, G. Martinez, M. Potemski, C. Berger, and W. A. de Heer, Magnetospectroscopy of epitaxial few-layer graphene, Solid State Commun. 143, 123 (2007).
  41. P. Kužel, H. Němec, F. Kadlec, and C. Kadlec, Gouy shift correction for highly accurate refractive index retrieval in time-domain terahertz spectroscopy, Opt. Express 18, 15338 (2010).
  42. V. Skoromets, H. Němec, V. Goian, S. Kamba, and P. Kužel, Performance comparison of time-domain terahertz, multiterahertz, and fourier transform infrared spectroscopies, J. Infrared Millim. Terahertz Waves 39, 1249 (2018).
  43. A. Singh, H. Němec, J. Kunc, and P. Kužel, Nanoscale terahertz conductivity and ultrafast dynamics of terahertz plasmons in periodic arrays of epitaxial graphene nanoribbons, Phys. Rev. Res. 6, 033063 (2024).
  44. K. L. Krewer, Z. Mics, J. Arabski, G. Schmerber, E. Beaurepaire, M. Bonn, and D. Turchinovich, Accurate terahertz spectroscopy of supported thin films by precise substrate thickness correction, Opt. Lett. 43, 447 (2018).
  45. L. Fekete, P. Kužel, H. Němec, F. Kadlec, A. Dejneka, J. Stuchlík, and A. Fejfar, Ultrafast carrier dynamics in microcrystalline silicon probed by time-resolved terahertz spectroscopy, Phys. Rev. B 79, 115306 (2009).
  46. H.-K. Nienhuys and V. Sundström, Intrinsic complications in the analysis of optical-pump, terahertz probe experiments, Phys. Rev. B 71, 235110 (2005).
  47. N. W. Ashcroft and N. D. Mermin, Solid State Physics (Holt, Rinehart and Winston, New York, 1976).
  48. E. H. Hwang and S. Das Sarma, Screening-induced temperature-dependent transport in two-dimensional graphene, Phys. Rev. B 79, 165404 (2009).
  49. H. Nemec, V. Zajac, I. Rychetsky, D. Fattakhova-Rohlfing, B. Mandlmeier, T. Bein, Z. Mics, and P. Kuzel, Charge transport in TiO2 films with complex percolation pathways investigated by time-resolved terahertz spectroscopy, IEEE Trans. Terahertz Sci. Technol. 3, 302 (2013).
  50. M. M. Jadidi, J. C. König-Otto, S. Winnerl, A. B. Sushkov, H. D. Drew, T. E. Murphy, and M. Mittendorff, Nonlinear terahertz absorption of graphene plasmons, Nano Lett. 16, 2734 (2016).
  51. K. W. Clark, X.-G. Zhang, I. V. Vlassiouk, G. He, R. M. Feenstra, and A.-P. Li, Spatially resolved mapping of electrical conductivity across individual domain (grain) boundaries in graphene, ACS Nano 7, 7956 (2013).
  52. A. Cvitkovic, N. Ocelic, and R. Hillenbrand, Analytical model for quantitative prediction of material contrasts in scattering-type near-field optical microscopy, Opt. Express, OE 15, 8550 (2007).
  53. P. Neugebauer, M. Orlita, C. Faugeras, A.-L. Barra, and M. Potemski, How perfect can graphene be? Phys. Rev. Lett. 103, 136403 (2009).
  54. N. M. R. Peres, F. Guinea, and A. H. Castro Neto, Electronic properties of disordered two-dimensional carbon, Phys. Rev. B 73, 125411 (2006).
  55. V. M. Pereira,J. M. B. Lopes dos Santos, and A. H. Castro, Neto, Modeling disorder in graphene, Phys. Rev. B 77, 115109 (2008).
  56. C.-P. Lu, M. Rodriguez-Vega, G. Li, A. Luican-Mayer, K. Watanabe, T. Taniguchi, E. Rossi, and E. Y. Andrei, Local, global, and nonlinear screening in twisted double-layer graphene, Proc. Natl. Acad. Sci. USA 113, 6623 (2016).
  57. S. V. Morozov, K. S. Novoselov, M. I. Katsnelson, F. Schedin, D. C. Elias, J. A. Jaszczak, and A. K. Geim, Giant intrinsic carrier mobilities in graphene and its bilayer, Phys. Rev. Lett. 100, 016602 (2008).
  58. B. A. Ruzicka, S. Wang, L. K. Werake, B. Weintrub, K. P. Loh, and H. Zhao, Hot carrier diffusion in graphene, Phys. Rev. B 82, 195414 (2010).
  59. D. Sun, Z.-K. Wu, C. Divin, X. Li, C. Berger, W. A. de Heer, P. N. First, and T. B. Norris, Ultrafast relaxation of excited Dirac fermions in epitaxial graphene using optical differential transmission spectroscopy, Phys. Rev. Lett. 101, 157402 (2008).
  60. K.-J. Tielrooij, et al., Out-of-plane heat transfer in van der Waals stacks through electron–hyperbolic phonon coupling, Nat. Nanotechnol. 13, 41 (2018).
  61. A. Singh, J. Kunc, T. Troha, H. Němec, and P. Kužel, Ultrafast terahertz photoconductivity and near-field imaging of nanoscale inhomogeneities in multilayer epitaxial graphene nanoribbons, https://doi.org/10.57680/asep.0640402.

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation