- Open Access
Ultrafast terahertz photoconductivity and near-field imaging of nanoscale inhomogeneities in multilayer epitaxial graphene nanoribbons
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 () 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 : the scattering time drops by an order of magnitude down to ∼10 fs upon an increase of from 50 K to , which is attributed to an enhanced electron-electron and electron-phonon scattering and to an interaction of electrons with mid-gap states.
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References (61)
- 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).
- 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).
- K. V. Emtsev, et al., Towards wafer-size graphene layers by atmospheric pressure graphitization of silicon carbide, Nat. Mater. 8, 203 (2009).
- 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).
- 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).
- 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).
- 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).
- 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).
- M. Sprinkle, et al., First Direct observation of a nearly ideal graphene band structure, Phys. Rev. Lett. 103, 226803 (2009).
- 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).
- J.-H. Chen, C. Jang, S. Xiao, M. Ishigami, and M. S. Fuhrer, Intrinsic and extrinsic performance limits of graphene devices on , Nat. Nanotechnol. 3, 206 (2008).
- E. H. Hwang and S. Das Sarma, Acoustic phonon scattering limited carrier mobility in two-dimensional extrinsic graphene, Phys. Rev. B 77, 115449 (2008).
- 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).
- 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).
- 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).
- Y.-M. Lin, et al., Multicarrier transport in epitaxial multilayer graphene, Appl. Phys. Lett. 97, 112107 (2010).
- W. A. de Heer, et al., Epitaxial graphene, Solid State Commun. 143, 92 (2007).
- 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).
- M. Mittendorff, et al., Carrier dynamics in Landau-quantized graphene featuring strong Auger scattering, Nat. Phys. 11, 75 (2015).
- 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).
- 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).
- J. W. Han, et al., Plasmonic terahertz nonlinearity in graphene disks, Adv. Photon. Res. 3, 2100218 (2022).
- S. D. Sarma, S. Adam, E. H. Hwang, and E. Rossi, Electronic transport in two-dimensional graphene, Rev. Mod. Phys. 83, 407 (2011).
- 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).
- P. Kužel and H. Němec, Terahertz spectroscopy of nanomaterials: A close look at charge-carrier transport, Adv. Opt. Mater. 8, 1900623 (2020).
- 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).
- A. Tomadin, et al., The ultrafast dynamics and conductivity of photoexcited graphene at different Fermi energies, Sci. Adv. 4, eaar5313 (2018).
- M. Massicotte, G. Soavi, A. Principi, and K.-J. Tielrooij, Hot carriers in graphene – fundamentals and applications, Nanoscale 13, 8376 (2021).
- 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).
- A. Singh and S. Kumar, Terahertz photonics and optoelectronics of carbon-based nanosystems, J. Appl. Phys. 131, 160901 (2022).
- A. Singh and S. Kumar, Phonon bottleneck in temperature-dependent hot carrier relaxation in graphene oxide, J. Phys. Chem. C 125, 26583 (2021).
- 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).
- 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).
- M. Koshino and T. Ando, Magneto-optical properties of multilayer graphene, Phys. Rev. B 77, 115313 (2008).
- M. Orlita, et al., Approaching the Dirac point in high-mobility multilayer epitaxial graphene, Phys. Rev. Lett. 101, 267601 (2008).
- 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).
- 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).
- 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).
- C. Berger, et al., Electronic confinement and coherence in patterned epitaxial graphene, Science 312, 1191 (2006).
- 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).
- 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).
- 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).
- 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).
- 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).
- 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).
- H.-K. Nienhuys and V. Sundström, Intrinsic complications in the analysis of optical-pump, terahertz probe experiments, Phys. Rev. B 71, 235110 (2005).
- N. W. Ashcroft and N. D. Mermin, Solid State Physics (Holt, Rinehart and Winston, New York, 1976).
- E. H. Hwang and S. Das Sarma, Screening-induced temperature-dependent transport in two-dimensional graphene, Phys. Rev. B 79, 165404 (2009).
- H. Nemec, V. Zajac, I. Rychetsky, D. Fattakhova-Rohlfing, B. Mandlmeier, T. Bein, Z. Mics, and P. Kuzel, Charge transport in films with complex percolation pathways investigated by time-resolved terahertz spectroscopy, IEEE Trans. Terahertz Sci. Technol. 3, 302 (2013).
- 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).
- 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).
- 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).
- P. Neugebauer, M. Orlita, C. Faugeras, A.-L. Barra, and M. Potemski, How perfect can graphene be? Phys. Rev. Lett. 103, 136403 (2009).
- N. M. R. Peres, F. Guinea, and A. H. Castro Neto, Electronic properties of disordered two-dimensional carbon, Phys. Rev. B 73, 125411 (2006).
- V. M. Pereira,J. M. B. Lopes dos Santos, and A. H. Castro, Neto, Modeling disorder in graphene, Phys. Rev. B 77, 115109 (2008).
- 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).
- 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).
- 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).
- 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).
- 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).
- 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.