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  • Letter
  • Open Access

Linearly dispersive bands at the onset of correlations in KxC60 films

Ping Ai1, Luca Moreschini1,2, Ryo Mori1, Drew W. Latzke1,2, Jonathan D. Denlinger3, Alex Zettl1,2,4, Claudia Ojeda-Aristizabal5, and Alessandra Lanzara1,2,*

  • 1Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA
  • 2Department of Physics, University of California, Berkeley, Berkeley, California 94720, USA
  • 3Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA
  • 4Kavli Energy NanoSciences Institute, Berkeley, California 94720, USA
  • 5Department of Physics and Astronomy, California State University, Long Beach, Long Beach, California 90840, USA

  • *alanzara@lbl.gov
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Phys. Rev. Research 5, L022042 – Published 30 May, 2023

DOI: https://doi.org/10.1103/PhysRevResearch.5.L022042

Abstract

Molecular crystals are a flexible platform to induce novel electronic phases. Due to the weak forces between molecules, intermolecular distances can be varied over larger ranges than interatomic distances in atomic crystals. On the other hand, the hopping terms are generally small, which results in narrow bands, strong correlations, and heavy electrons. Here, by growing KxC60 fullerides on hexagonal layered Bi2Se3, we show that upon doping the series undergoes a Mott transition from a molecular insulator to a correlated metal and an in-gap state evolves into highly dispersive Dirac-like fermions at half filling, where superconductivity occurs. This picture challenges the commonly accepted description of the low-energy quasiparticles as appearing from a gradual electron doping of the conduction states and suggests an intriguing parallel with the more famous family of the cuprate superconductors. More in general, it indicates that molecular crystals offer a viable route to engineer electron-electron interactions.

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References (56)

  1. M. Kiguchi, K.-i. Iizumi, K. Saiki, and A. Koma, Atomic and electronic structures of heteroepitaxial C60 film grown on Ni(1 1 1), Cu(1 1 1), Appl. Surf. Sci. 212–213, 101 (2003).
  2. L.-L. Wang and H.-P. Cheng, Rotation, translation, charge transfer, and electronic structure of C60 on Cu(111) surface, Phys. Rev. B 69, 045404 (2004).
  3. K. Kim, T. H. Lee, E. J. G. Santos, P. S. Jo, A. Salleo, Y. Nishi, and Z. Bao, Structural and electrical investigation of C60−graphene vertical heterostructures, ACS Nano 9, 5922 (2015).
  4. C. Ojeda-Aristizabal, E. J. G. Santos, S. Onishi, A. Yan, H. I. Rasool, S. Kahn, Y. Lv, D. W. Latzke, J. Velasco, M. F. Crommie, M. Sorensen, K. Gotlieb, C.-Y. Lin, K. Watanabe, T. Taniguchi, A. Lanzara, and A. Zettl, Molecular arrangement and charge transfer in C60/graphene heterostructures, ACS Nano 11, 4686 (2017).
  5. N. Haag, D. Lüftner, F. Haag, J. Seidel, L. L. Kelly, G. Zamborlini, M. Jugovac, V. Feyer, M. Aeschlimann, P. Puschnig, M. Cinchetti, and B. Stadtmüller, Signatures of an atomic crystal in the band structure of a C60 thin film, Phys. Rev. B 101, 165422 (2020).
  6. Y. Cao, V. Fatemi, A. Demir, S. Fang, S. L. Tomarken, J. Y. Luo, J. D. Sanchez-Yamagishi, K. Watanabe, T. Taniguchi, and E. Kaxiras, Correlated insulator behaviour at half-filling in magic-angle graphene superlattices, Nature (London) 556, 80 (2018).
  7. Y. Cao, V. Fatemi, S. Fang, K. Watanabe, T. Taniguchi, E. Kaxiras, and P. Jarillo-Herrero, Unconventional superconductivity in magic-angle graphene superlattices, Nature (London) 556, 43 (2018).
  8. M. M. Ugeda, A. J. Bradley, S.-F. Shi, H. Felipe, Y. Zhang, D. Y. Qiu, W. Ruan, S.-K. Mo, Z. Hussain, Z.-X. Shen, Giant bandgap renormalization and excitonic effects in a monolayer transition metal dichalcogenide semiconductor, F. Wang, S. G. Louie, and M. F. Crommie, Nat. Mater. 13, 1091 (2014).
  9. L. Wang, E.-M. Shih, A. Ghiotto, L. Xian, D. A. Rhodes, C. Tan, M. Claassen, D. M. Kennes, Y. Bai, B. Kim, K. Watanabe, T. Taniguchi, X. Zhu, J. Hone, A. Rubio, A. N. Pasupathy, and C. R. Dean, Correlated electronic phases in twisted bilayer transition metal dichalcogenides, Nat. Mater. 19, 861 (2020).
  10. Y. Xu, C. Horn, J. Zhu, Y. Tang, L. Ma, L. Li, S. Liu, K. Watanabe, T. Taniguchi, J. C. Hone, J. Shan, and K. F. Mak, Creation of moiré bands in a monolayer semiconductor by spatially periodic dielectric screening, Nat. Mater. 20, 645 (2021).
  11. O. Gunnarsson, Superconductivity in fullerides, Rev. Mod. Phys. 69, 575 (1997).
  12. M. Capone, M. Fabrizio, C. Castellani, and E. Tosatti, Colloquium: Modeling the unconventional superconducting properties of expanded A3C60 fullerides, Rev. Mod. Phys. 81, 943 (2009).
  13. Y. Takabayashi and K. Prassides, Unconventional high-Tc superconductivity in fullerides, Philos. Trans. R. Soc. A 374, 20150320 (2016).
  14. M. Capone, M. Fabrizio, C. Castellani, and E. Tosatti, Strongly correlated superconductivity, Science 296, 2364 (2002).
  15. P. Durand, G. R. Darling, Y. Dubitsky, A. Zaopo, and M. J. Rosseinsky, The MottHubbard insulating state and orbital degeneracy in the superconducting C603− fulleride family, Nat. Mater. 2, 605 (2003).
  16. N. Manini and E. Tosatti, Theoretical aspects of highly correlated fullerides: metal-insulator transition, arXiv:cond-mat/0602134.
  17. F. Steglich and S. Wirth, Foundations of heavy-fermion superconductivity: Lattice Kondo effect and Mott physics, Rep. Prog. Phys. 79, 084502 (2016).
  18. H. M. Yamamoto, Phase-transition devices based on organic Mott insulators, Bull. Chem. Soc. Jpn. 94, 2505 (2021).
  19. C. T. Chen, L. Tjeng, P. Rudolf, G. Meigs, J. Rowe, J. Chen, J. McCauley, A. Smith, A. McGhie, and W. Romanow, Electronic states and phases of KxC60 from photoemission and X-ray absorption spectroscopy, Nature (London) 352, 603 (1991).
  20. M. Merkel, M. Knupfer, M. S. Golden, J. Fink, R. Seemann, and R. L. Johnson, Photoemission study of the electronic structure of C60 and KxC60, Phys. Rev. B 47, 11470 (1993).
  21. G. K. Wertheim and D. N. E. Buchanan, Bulk and surface electronic structures of potassium fullerides, Phys. Rev. B 47, 12912 (1993).
  22. J. L. McChesney, A. Bostwick, T. Ohta, T. Seyller, K. Horn, J. González, and E. Rotenberg, Extended van Hove Singularity and Superconducting Instability in Doped Graphene, Phys. Rev. Lett. 104, 136803 (2010).
  23. C. Hwang, D. A. Siegel, S.-K. Mo, W. Regan, A. Ismach, Y. Zhang, A. Zettl, and A. Lanzara, Fermi velocity engineering in graphene by substrate modification, Sci. Rep. 2, 590 (2012).
  24. S. Kawasaki, J. Fukui, T. Motoyama, Y. Suzuki, S. Shibasaki, and G.-q. Zheng, The Mott state and superconductivity in face-centred cubic structured Cs3C60: A Cs133-nuclear magnetic resonance study under pressure, J. Phys. Soc. Jpn. 82, 014709 (2013).
  25. V. Brouet, W. Yang, X. Zhou, Z. Hussain, and Z. Shen, Dependence of the band structure of C60 monolayers on molecular orientations and doping observed by angle resolved photoemission, J. Phys. Chem. Solids 67, 218 (2006).
  26. R. Hesper, L. H. Tjeng, A. Heeres, and G. A. Sawatzky, Photoemission evidence of electronic stabilization of polar surfaces in K3C60, Phys. Rev. B 62, 16046 (2000).
  27. W. Yang, V. Brouet, X. Zhou, H. J. Choi, S. G. Louie, M. L. Cohen, S. Kellar, P. Bogdanov, A. Lanzara, and A. Goldoni, Band structure and fermi surface of electron-doped C60 monolayers, Science 300, 303 (2003).
  28. V. Brouet, W. L. Yang, X. J. Zhou, H. J. Choi, S. G. Louie, M. L. Cohen, A. Goldoni, F. Parmigiani, Z. Hussain, and Z. X. Shen, Orientation-Dependent C60 Electronic Structures Revealed by Photoemission Spectroscopy, Phys. Rev. Lett. 93, 197601 (2004).
  29. W. W. Pai, H. T. Jeng, C.-M. Cheng, C.-H. Lin, X. Xiao, A. Zhao, X. Zhang, G. Xu, X. Q. Shi, M. A. Van Hove, C.-S. Hsue, and K.-D. Tsuei, Optimal Electron Doping of a C60 Monolayer on Cu(111) via Interface Reconstruction, Phys. Rev. Lett. 104, 036103 (2010).
  30. See Supplemental Material at http://link.aps.org/supplemental/10.1103/PhysRevResearch.5.L022042 for materials and methods, additional characterization data and a summary of reported reconstructions of C60 on various substrates.
  31. D. W. Latzke, C. Ojeda-Aristizabal, S. M. Griffin, J. D. Denlinger, J. B. Neaton, A. Zettl, and A. Lanzara, Observation of highly dispersive bands in pure thin film C60, Phys. Rev. B 99, 045425 (2019).
  32. P. W. Stephens, L. Mihaly, P. L. Lee, R. L. Whetten, S.-M. Huang, R. Kaner, F. Deiderich, and K. Holczer, Structure of single-phase superconducting K3C60, Nature (London) 351, 632 (1991).
  33. J. L. Martins and N. Troullier, Structural and electronic properties of KnC60, Phys. Rev. B 46, 1766 (1992).
  34. Q. Zhu, D. E. Cox, and J. E. Fischer, Phase transitions in KC60: Dimer formation via rapid quenching, Phys. Rev. B 51, 3966 (1995).
  35. G. Oszlányi, G. Bortel, G. Faigel, M. Tegze, L. Gránásy, S. Pekker, P. W. Stephens, G. Bendele, R. Dinnebier, G. Mihály, A. Jánossy, O. Chauvet, and L. Forró, Dimerization in KC60 and RbC60, Phys. Rev. B 51, 12228 (1995).
  36. T. Pichler, M. Knupfer, M. S. Golden, S. Haffner, R. Friedlein, J. Fink, W. Andreoni, A. Curioni, M. Keshavarz-K, C. Bellavia-Lund, A. Sastre, J.-C. Hummelen, and F. Wudl, On-Ball Doping of Fullerenes: The Electronic Structure of C59N Dimers from Experiment and Theory, Phys. Rev. Lett. 78, 4249 (1997).
  37. R. Macovez, P. Rudolf, I. Marenne, L. Kjeldgaard, P. A. Brühwiler, T. Pichler, P. Vilmercati, R. Larciprete, L. Petaccia, G. Bertoni, and A. Goldoni, Electronic surface reconstruction and correlation in the fcc and dimer phases of RbC60, Phys. Rev. B 75, 195424 (2007).
  38. D. Konarev, S. Khasanov, A. Otsuka, M. Maesato, G. Saito, and R. Lyubovskaya, A two-dimensional organic metal based on fullerene, Angew. Chem. Int. Ed. 49, 4829 (2010).
  39. S. C. Erwin and W. E. Pickett, Theoretical fermi-surface properties and superconducting parameters for K3C60, Science 254, 842 (1991).
  40. O. Gunnarsson, E. Koch, and R. M. Martin, Mott transition in degenerate Hubbard models: Application to doped fullerenes, Phys. Rev. B 54, R11026 (1996).
  41. J. E. Han, E. Koch, and O. Gunnarsson, Metal-Insulator Transitions: Influence of Lattice Structure, Jahn-Teller Effect, and Hund's Rule Coupling, Phys. Rev. Lett. 84, 1276 (2000).
  42. S. Satpathy, V. P. Antropov, O. K. Andersen, O. Jepsen, O. Gunnarsson, and A. I. Liechtenstein, Conduction-band structure of alkali-metal-doped C60, Phys. Rev. B 46, 1773 (1992).
  43. Y. Wang, Y. He, K. Wohlfeld, M. Hashimoto, E. W. Huang, D. Lu, S.-K. Mo, S. Komiya, C. Jia, B. Moritz, Z.-X. Shen, and T. P. Devereaux, Emergence of quasiparticles in a doped Mott insulator, Commun. Phys. 3, 210 (2020).
  44. D. W. Latzke, C. Ojeda-Aristizabal, J. D. Denlinger, R. Reno, A. Zettl, and A. Lanzara, Orbital character effects in the photon energy and polarization dependence of pure C60 photoemission, ACS Nano 13, 12710 (2019).
  45. A. H. Castro Neto, F. Guinea, N. M. R. Peres, K. S. Novoselov, and A. K. Geim, The electronic properties of graphene, Rev. Mod. Phys. 81, 109 (2009).
  46. Y. Xia, D. Qian, D. Hsieh, L. Wray, A. Pal, H. Lin, A. Bansil, D. Grauer, Y. S. Hor, R. J. Cava, and M. Z. Hasan, Observation of a large-gap topological-insulator class with a single Dirac cone on the surface, Nat. Phys. 5, 398 (2009).
  47. M. König, S. Wiedmann, C. Brüne, A. Roth, H. Buhmann, L. W. Molenkamp, X.-L. Qi, and S.-C. Zhang, Quantum spin Hall insulator state in HgTe quantum wells, Science 318, 766 (2007).
  48. P. Zhang, K. Yaji, T. Hashimoto, Y. Ota, T. Kondo, K. Okazaki, Z. Wang, J. Wen, G. D. Gu, H. Ding, and S. Shin, Observation of topological superconductivity on the surface of an iron-based superconductor, Science 360, 182 (2018).
  49. S. Borisenko, Q. Gibson, D. Evtushinsky, V. Zabolotnyy, B. Büchner, and R. J. Cava, Experimental Realization of a Three-Dimensional Dirac Semimetal, Phys. Rev. Lett. 113, 027603 (2014).
  50. M. Neupane, S.-Y. Xu, R. Sankar, N. Alidoust, G. Bian, C. Liu, I. Belopolski, T.-R. Chang, H.-T. Jeng, H. Lin, A. Bansil, F. Chou, and M. Z. Hasan, Observation of a three-dimensional topological Dirac semimetal phase in high-mobility Cd3As2, Nat. Commun. 5, 3786 (2014).
  51. Z. K. Liu, B. Zhou, Y. Zhang, Z. J. Wang, H. M. Weng, D. Prabhakaran, S.-K. Mo, Z. X. Shen, Z. Fang, X. Dai, Z. Hussain, and Y. L. Chen, Discovery of a three-dimensional topological dirac semimetal, Na3Bi, Science 343, 864 (2014).
  52. M.-Q. Ren, S. Han, S.-Z. Wang, J.-Q. Fan, C.-L. Song, X.-C. Ma, and Q.-K. Xue, Direct Observation of Full-Gap Superconductivity and Pseudogap in Two-Dimensional Fullerides, Phys. Rev. Lett. 124, 187001 (2020).
  53. S. Zhou, G.-H. Gweon, J. Graf, A. Fedorov, C. Spataru, R. Diehl, Y. Kopelevich, D.-H. Lee, S. G. Louie, and A. Lanzara, First direct observation of Dirac fermions in graphite, Nat. Phys. 2, 595 (2006).
  54. R. W. Lof, M. A. van Veenendaal, B. Koopmans, H. T. Jonkman, and G. A. Sawatzky, Band gap, excitons, and Coulomb interaction in solid C60, Phys. Rev. Lett. 68, 3924 (1992).
  55. L. Hou, X. Cui, B. Guan, S. Wang, R. Li, Y. Liu, D. Zhu, and J. Zheng, Synthesis of a monolayer fullerene network, Nature (London) 606, 507 (2022).
  56. E. Meirzadeh, A. M. Evans, M. Rezaee, M. Milich, C. J. Dionne, T. P. Darlington, S. T. Bao, A. K. Bartholomew, T. Handa, D. J. Rizzo, R. A. Wiscons, M. Reza, A. Zangiabadi, N. Fardian-Melamed, A. C. Crowther, P. J. Schuck, D. N. Basov, X. Zhu, A. Giri, P. E. Hopkins et al., A few-layer covalent network of fullerenes, Nature (London) 613, 71 (2023).

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Phys. Rev. Research 5, L022042– Published 30 May, 2023
  • Received 1 September 2022
  • Revised 18 March 2023
  • Accepted 26 April 2023
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