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  • Letter
  • Open Access

Ultrafast charge separation induced by a uniform field in graphene nanoribbons

Jan-Philip Joost* and Michael Bonitz

  • *Contact author: joost@theo-physik.uni-kiel.de
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Phys. Rev. Research 7, L032068 – Published 23 September, 2025

DOI: https://doi.org/10.1103/dtk9-xv6n

Abstract

When heteronuclear molecules are illuminated by light of spatially uniform intensity, electronic excitations may, nevertheless, be restricted to parts of the system, depending on the absorption properties of its constituents. Here, we show that this effect is observed also in homogeneous carbon-based systems, such as graphene nanoribbons (GNRs): A spatially uniform laser pulse can create strongly localized carrier excitations, including excitons, on the subnanometer scale within a few femtoseconds. The origin of this effect is the unusual topological-based electronic structure of the GNRs. This opens exciting avenues for nanoelectronics and brings petahertz switching within reach. Using nonequilibrium Green’s function simulations, we demonstrate this effect by exciting small GNR heterostructures of suitable geometry with a laser pulse with carefully chosen photon energy, polarization, and carrier-envelope phase.

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References (59)

  1. T. Rybka, M. Ludwig, M. F. Schmalz, V. Knittel, D. Brida, and A. Leitenstorfer, Sub-cycle optical phase control of nanotunnelling in the single-electron regime, Nat. Photon. 10, 667 (2016).
  2. P. D. Keathley, W. P. Putnam, P. Vasireddy, R. G. Hobbs, Y. Yang, K. K. Berggren, and F. X. Kärtner, Vanishing carrier-envelope-phase-sensitive response in optical-field photoemission from plasmonic nanoantennas, Nat. Phys. 15, 1128 (2019).
  3. T. Boolakee, C. Heide, A. Garzón-Ramirez, H. B. Weber, I. Franco, and P. Hommelhoff, Light-field control of real and virtual charge carriers, Nature (London) 605, 251 (2022).
  4. S. Meier, J. Heimerl, and P. Hommelhoff, Few-electron correlations after ultrafast photoemission from nanometric needle tips, Nat. Phys. 19, 1402 (2023).
  5. J. Pettine, P. Padmanabhan, T. Shi, L. Gingras, L. McClintock, C.-C. Chang, K. W. C. Kwock, L. Yuan, Y. Huang, J. Nogan, J. K. Baldwin, P. Adel, R. Holzwarth, A. K. Azad, F. Ronning, A. J. Taylor, R. P. Prasankumar, S.-Z. Lin, and H.-T. Chen, Light-driven nanoscale vectorial currents, Nature (London) 626, 984 (2024).
  6. G. Inzani, L. Adamska, A. Eskandari-asl, N. Di Palo, G. L. Dolso, B. Moio, L. J. D’Onofrio, A. Lamperti, A. Molle, R. Borrego-Varillas, M. Nisoli, S. Pittalis, C. A. Rozzi, A. Avella, and M. Lucchini, Field-driven attosecond charge dynamics in germanium, Nat. Photon. 17, 1059 (2023).
  7. A. Chernikov, T. C. Berkelbach, H. M. Hill, A. Rigosi, Y. Li, B. Aslan, D. R. Reichman, M. S. Hybertsen, and T. F. Heinz, Exciton binding energy and nonhydrogenic Rydberg series in monolayer WS2, Phys. Rev. Lett. 113, 076802 (2014).
  8. G. Moody, C. Kavir Dass, K. Hao, C.-H. Chen, L.-J. Li, A. Singh, K. Tran, G. Clark, X. Xu, G. Berghäuser, E. Malic, A. Knorr, and X. Li, Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides, Nat. Commun. 6, 8315 (2015).
  9. M. X. Na and Z. Ye, Probing the dark side of the exciton, Science 370, 1166 (2020).
  10. G. Wang, A. Chernikov, M. M. Glazov, T. F. Heinz, X. Marie, T. Amand, and B. Urbaszek, Colloquium: Excitons in atomically thin transition metal dichalcogenides, Rev. Mod. Phys. 90, 021001 (2018).
  11. S. Jiang, T. Neuman, A. Boeglin, F. Scheurer, and G. Schull, Topologically localized excitons in single graphene nanoribbons, Science 379, 1049 (2023).
  12. M. Fujita, K. Wakabayashi, K. Nakada, and K. Kusakabe, Peculiar localized state at zigzag graphite edge, J. Phys. Soc. Jpn. 65, 1920 (1996).
  13. Y.-W. Son, M. L. Cohen, and S. G. Louie, Energy gaps in graphene nanoribbons, Phys. Rev. Lett. 97, 216803 (2006).
  14. M. El Abbassi, M. L. Perrin, G. B. Barin, S. Sangtarash, J. Overbeck, O. Braun, C. J. Lambert, Q. Sun, T. Prechtl, A. Narita, K. Müllen, P. Ruffieux, H. Sadeghi, R. Fasel, and M. Calame, Controlled quantum dot formation in atomically engineered graphene nanoribbon field-effect transistors, ACS Nano 14, 5754 (2020).
  15. H. Wang, H. S. Wang, C. Ma, L. Chen, C. Jiang, C. Chen, X. Xie, A.-P. Li, and X. Wang, Graphene nanoribbons for quantum electronics, Nat. Rev. Phys. 3, 791 (2021).
  16. Y. Gu, Z. Qiu, and K. Müllen, Nanographenes and graphene nanoribbons as multitalents of present and future materials science, J. Am. Chem. Soc. 144, 11499 (2022).
  17. D. Prezzi, D. Varsano, A. Ruini, A. Marini, and E. Molinari, Optical properties of graphene nanoribbons: The role of many-body effects, Phys. Rev. B 77, 041404 (2008).
  18. J.-P. Joost, A.-P. Jauho, and M. Bonitz, Correlated topological states in graphene nanoribbon heterostructures, Nano Lett. 19, 9045 (2019).
  19. L. Yang, M. L. Cohen, and S. G. Louie, Excitonic effects in the optical spectra of graphene nanoribbons, Nano Lett. 7, 3112 (2007).
  20. R. E. Blackwell, F. Zhao, E. Brooks, J. Zhu, I. Piskun, S. Wang, A. Delgado, Y.-L. Lee, S. G. Louie, and F. R. Fischer, Spin splitting of dopant edge state in magnetic zigzag graphene nanoribbons, Nature (London) 600, 647 (2021).
  21. S. Song, Y. Teng, W. Tang, Z. Xu, Y. He, J. Ruan, T. Kojima, W. Hu, F. J. Giessibl, H. Sakaguchi, S. G. Louie, and J. Lu, Janus graphene nanoribbons with localized states on a single zigzag edge, Nature (London) 637, 580 (2025).
  22. H. Abdelslam, D. Corna, R. B. Payod, M. A. Sakr, O. H. Abd-Elkader, Q. Zhang, and V. A. Saroka, Topological junction states in graphene nanoribbons: A route to topological chemistry, Nano Lett. 25, 10594 (2025).
  23. D. J. Rizzo, G. Veber, T. Cao, C. Bronner, T. Chen, F. Zhao, H. Rodriguez, S. G. Louie, M. F. Crommie, and F. R. Fischer, Topological band engineering of graphene nanoribbons, Nature (London) 560, 204 (2018).
  24. K. Slicker, A. Delgado, J. Jiang, W. Tang, A. Cronin, R. E. Blackwell, S. G. Louie, and F. R. Fischer, Engineering small HOMO-LUMO gaps in polycyclic aromatic hydrocarbons with topologically protected states, Nano Lett. 24, 5387 (2024).
  25. R. Wang, F. Bi, W. Lu, X. Zheng, and C. Yam, Enhancement of laser pulse induced photocurrents by topological states in graphene nanoribbons, Phys. Rev. B 109, 195303 (2024).
  26. F. Fassioli, R. Dinshaw, P. C. Arpin, and G. D. Scholes, Photosynthetic light harvesting: Excitons and coherence, J. R. Soc. Interface 11, 20130901 (2014).
  27. M. W. Doherty, N. B. Manson, P. Delaney, F. Jelezko, J. Wrachtrup, and L. C. Hollenberg, The nitrogen-vacancy colour centre in diamond, Phys. Rep. 528, 1 (2013).
  28. G. Chiappe, E. Louis, E. San-Fabián, and J. A. Vergés, Can model Hamiltonians describe the electron–electron interaction in π-conjugated systems? PAH and graphene, J. Phys.: Condens. Matter 27, 463001 (2015).
  29. K. Ohno, Some remarks on the Pariser-Parr-Pople method, Theor. Chim. Acta 2, 219 (1964).
  30. J. A. Vergés, E. SanFabián, G. Chiappe, and E. Louis, Fit of Pariser-Parr-Pople and Hubbard model Hamiltonians to charge and spin states of polycyclic aromatic hydrocarbons, Phys. Rev. B 81, 085120 (2010).
  31. J.-P. Joost, Green functions approach to graphene nanostructures, Ph.D. thesis, Christian-Albrechts-Universität zu Kiel, Kiel, 2022, https://nbn-resolving.org/urn:nbn:de:gbv:8:3-2023-00427-4.
  32. J.-P. Joost, N. Schlünzen, and M. Bonitz, Femtosecond electron dynamics in graphene nanoribbons—A nonequilibrium Green functions approach within an extended Hubbard model, Phys. Status Solidi (b) 256, 1800498 (2019).
  33. See Supplemental Material at http://link.aps.org/supplemental/10.1103/dtk9-xv6n for details on the theoretical description of the nanostructures using the PPP model and the G1-G2 scheme.
  34. N. Schlünzen, J.-P. Joost, and M. Bonitz, Achieving the scaling limit for nonequilibrium Green functions simulations, Phys. Rev. Lett. 124, 076601 (2020).
  35. J.-P. Joost, N. Schlünzen, and M. Bonitz, G1-G2 scheme: Dramatic acceleration of nonequilibrium Green functions simulations within the Hartree-Fock generalized Kadanoff-Baym ansatz, Phys. Rev. B 101, 245101 (2020).
  36. M. Bonitz, C. Makait, E. Schroedter, T. Kalsberger, J.-P. Joost, and K. Balzer, Accelerating nonequilibrium Green function simulations: The G1-G2 scheme and beyond, Phys. Status Solidi (b) 261, 2300578 (2024).
  37. J.-P. Joost, N. Schlünzen, H. Ohldag, M. Bonitz, F. Lackner, and I. Brezinova, The dynamically screened ladder approximation: Simultaneous treatment of strong electronic correlations and dynamical screening out of equilibrium, Phys. Rev. B 105, 165155 (2022).
  38. T. Koopmans, Über die Zuordnung von Wellenfunktionen und Eigenwerten zu den Einzelnen Elektronen Eines Atoms, Physica 1, 104 (1934).
  39. A. Niggas, J. Schwestka, K. Balzer, D. Weichselbaum, N. Schlünzen, R. Heller, S. Creutzburg, H. Inani, M. Tripathi, C. Speckmann, N. McEvoy, T. Susi, J. Kotakoski, Z. Gan, A. George, A. Turchanin, M. Bonitz, F. Aumayr, and R. A. Wilhelm, Ion-induced surface charge dynamics in freestanding monolayers of graphene and MoS2 probed by the emission of electrons, Phys. Rev. Lett. 129, 086802 (2022).
  40. D. J. Rizzo, J. Jiang, D. Joshi, G. Veber, C. Bronner, R. A. Durr, P. H. Jacobse, T. Cao, A. Kalayjian, H. Rodriguez, P. Butler, T. Chen, S. G. Louie, F. R. Fischer, and M. F. Crommie, Rationally designed topological quantum dots in bottom-up graphene nanoribbons, ACS Nano 15, 20633 (2021).
  41. E. Louis, G. Chiappe, J. A. Vergés, and E. San-Fabián, Long-range effects in topologically defective arm-chair graphene nanoribbons, Nanomaterials 14, 778 (2024).
  42. I. Franco and P. Brumer, Minimum requirements for laser-induced symmetry breaking in quantum and classical mechanics, J. Phys. B: At. Mol. Opt. Phys. 41, 074003 (2008).
  43. A. Schiffrin, T. Paasch-Colberg, N. Karpowicz, V. Apalkov, D. Gerster, S. Mühlbrandt, M. Korbman, J. Reichert, M. Schultze, S. Holzner, J. V. Barth, R. Kienberger, R. Ernstorfer, V. S. Yakovlev, M. I. Stockman, and F. Krausz, Optical-field-induced current in dielectrics, Nature (London) 493, 70 (2013).
  44. Y.-L. Lee, F. Zhao, T. Cao, J. Ihm, and S. G. Louie, Topological phases in cove-edged and chevron graphene nanoribbons: Geometric structures, Z2 invariants, and junction states, Nano Lett. 18, 7247 (2018).
  45. F. M. Arnold, T.-J. Liu, A. Kuc, and T. Heine, Structure-imposed electronic topology in cove-edged graphene nanoribbons, Phys. Rev. Lett. 129, 216401 (2022).
  46. S. Mishra, D. Beyer, K. Eimre, S. Kezilebieke, R. Berger, O. Gröning, C. A. Pignedoli, K. Müllen, P. Liljeroth, P. Ruffieux, X. Feng, and R. Fasel, Topological frustration induces unconventional magnetism in a nanographene, Nat. Nanotechnol. 15, 22 (2020).
  47. S. Mishra, G. Catarina, F. Wu, R. Ortiz, D. Jacob, K. Eimre, J. Ma, C. A. Pignedoli, X. Feng, P. Ruffieux, J. Fernández-Rossier, and R. Fasel, Observation of fractional edge excitations in nanographene spin chains, Nature (London) 598, 287 (2021).
  48. Q. Sun, H. Jiang, Y. Yan, R. Fasel, and P. Ruffieux, Molecular heterostructure by fusing graphene nanoribbons of different lengths through a pentagon ring junction, Nano Res. 15, 8465 (2022).
  49. G. B. Barin, M. Di Giovannantonio, T. G. Lohr, S. Mishra, A. Kinikar, M. L. Perrin, J. Overbeck, M. Calame, X. Feng, R. Fasel, and P. Ruffieux, On-surface synthesis and characterization of teranthene and hexanthene: Ultrashort graphene nanoribbons with mixed armchair and zigzag edges, Nanoscale 15, 16766 (2023).
  50. The electron-hole PCF is defined as g¯ehα(r)=(1Nsitesα)∑R∈αgeh(r;R), where r and R are, respectively, relative and center-of-mass coordinates of the pair, and the sum (averaging) runs over the system part α.
  51. Y. Pavlyukh, E. Perfetto, D. Karlsson, R. van Leeuwen, and G. Stefanucci, Time-linear scaling nonequilibrium Green’s function methods for real-time simulations of interacting electrons and bosons. I. Formalism, Phys. Rev. B 105, 125134 (2022).
  52. Y. Pavlyukh, E. Perfetto, D. Karlsson, R. van Leeuwen, and G. Stefanucci, Time-linear scaling nonequilibrium Green’s function method for real-time simulations of interacting electrons and bosons. II. Dynamics of polarons and doublons, Phys. Rev. B 105, 125135 (2022).
  53. Y. Pavlyukh, R. Tuovinen, E. Perfetto, and G. Stefanucci, Cheers: A linear-scaling KBE+GKBA code, Phys. Status Solidi (b) 261, 2300504 (2024).
  54. X. Yao, W. Zheng, S. Osella, Z. Qiu, S. Fu, D. Schollmeyer, B. Müller, D. Beljonne, M. Bonn, H. I. Wang, K. Müllen, and A. Narita, Synthesis of nonplanar graphene nanoribbon with fjord edges, J. Am. Chem. Soc. 143, 5654 (2021).
  55. W. Niu, Y. Fu, G. Serra, K. Liu, J. Droste, Y. Lee, Z. Ling, F. Xu, J. D. Cojal González, A. Lucotti, J. P. Rabe, M. Ryan Hansen, W. Pisula, P. W. M. Blom, C.-A. Palma, M. Tommasini, Y. Mai, J. Ma, and X. Feng, Bottom-up solution synthesis of graphene nanoribbons with precisely engineered nanopores, Angew. Chem. Int. Ed. 62, e202305737 (2023).
  56. K. Liu, W. Zheng, S. Osella, Z.-L. Qiu, S. Böckmann, W. Niu, L. Meingast, H. Komber, S. Obermann, R. Gillen, M. Bonn, M. R. Hansen, J. Maultzsch, H. I. Wang, J. Ma, and X. Feng, Cove-edged chiral graphene nanoribbons with chirality-dependent bandgap and carrier mobility, J. Am. Chem. Soc. 146, 1026 (2024).
  57. A. Filinov, N. V. Prokof'ev, and M. Bonitz, Berezinskii-Kosterlitz-Thouless transition in two-dimensional dipole systems, Phys. Rev. Lett. 105, 070401 (2010).
  58. V. M. Pereira, Topological excitons, Nat. Phys. 18, 6 (2022).
  59. J. Cutshall, F. Mahdikhany, A. Roche, D. N. Shanks, M. R. Koehler, D. G. Mandrus, T. Taniguchi, K. Watanabe, Q. Zhu, B. J. LeRoy, and J. R. Schaibley, Imaging interlayer exciton superfluidity in a 2D semiconductor heterostructure, Sci. Adv. 11, eadr1772 (2025).

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Phys. Rev. Research 7, L032068– Published 23 September, 2025
  • Received 15 February 2025
  • Accepted 17 August 2025
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