- Open Access
Electronic structure reconstruction for charge density wave in heavily Cu-intercalated revealed by spatially resolved photoemission spectroscopy
Phys. Rev. B 113, 035146 – Published 23 January, 2026
DOI: https://doi.org/10.1103/dg1f-hm99
Abstract
Scanning photoemission microscopy (SPEM) and angle-resolved photoemission spectroscopy (ARPES) are used to investigate the electronic structure of across the charge density wave (CDW) transition. The electronic structure is found to be largely homogeneous in the normal state above the CDW transition. The ARPES measurements using a submicron beam size reveal a large electronlike pocket due to the Ti 3d band at the point while the Se band at the point is absent due to electron doping by the intercalated Cu. We have observed Fermi surface reconstruction below the CDW transition, in which Ti bands are folded into a reconstructed BZ rotated by , making the and points equivalent. The results demonstrate the presence of a CDW phase in the electronic structure of heavily Cu-intercalated . The findings reveal a platform for investigating the two-dimensional electronic phase in 1T- chalcogenides, which exhibit a unique interplay between CDW, superconductivity, and excitonic/lattice instabilities.
Physics Subject Headings (PhySH)
Article Text
Supplemental Material
References (53)
- J. Wilson, F. Di Salvo, and S. Mahajan, Charge-density waves and superlattices in the metallic layered transition metal dichalcogenides, Adv. Phys. 24, 117 (1975).
- K. Rahnejat, C. Howard, N. Shuttleworth, S. Schofield, K. Iwaya, C. Hirjibehedin, C. Renner, G. Aeppli, and M. Ellerby, Charge density waves in the graphene sheets of the superconductor , Nat. Commun. 2, 558 (2011).
- C. Howald, H. Eisaki, N. Kaneko, and A. Kapitulnik, Coexistence of periodic modulation of quasiparticle states and superconductivity in , Proc. Natl. Acad. Sci. USA 100, 9705 (2003).
- J. Chang, E. Blackburn, A. Holmes, N. Christensen, J. Larsen, J. Mesot, R. Liang, D. Bonn, W. N. Hardy, A. Watenphul, M. v. Zimmermann, E. M. Forgan, and S. M. Hayden, Direct observation of competition between superconductivity and charge density wave order in , Nat. Phys. 8, 871 (2012).
- G. Ghiringhelli, M. Le Tacon, M. Minola, S. Blanco-Canosa, C. Mazzoli, N. Brookes, G. De Luca, A. Frano, D. Hawthorn, F. He, T. Loew, M. Moretti Sala, D. C. Peets, M. Saluzzo, E. Schierle, R. Sutarto, G. A. Sawatzky, E. Weschke, B. Keimer, et al., Long-range incommensurate charge fluctuations in (Y, Nd), Science 337, 821 (2012).
- E. Rosenthal, E. Andrade, C. Arguello, R. Fernandes, L. Xing, X. Wang, C. Jin, A. Millis, and A. Pasupathy, Visualization of electron nematicity and unidirectional antiferroic fluctuations at high temperatures in NaFeAs, Nat. Phys. 10, 225 (2014).
- B. Keimer, S. Kivelson, M. Norman, S. Uchida, and J. Zaanen, From quantum matter to high-temperature superconductivity in copper oxides, Nature (London) 518, 179 (2015).
- M. Huber, Y. Lin, N. Dale, R. Sailus, S. Tongay, R. Kaindl, and A. Lanzara, Mapping the dispersion of the occupied and unoccupied band structure in photoexcited 1T-, J. Phys. Chem. Solids 168, 110740 (2022).
- M. Hattori, G. Tomassucci, G. Hayashi, M. Okawa, M. Kopciuszynski, A. Barinov, Y. Lu, H. Takagi, N. Saini, and T. Mizokawa, Robustness of excitonic coupling in against electronic inhomogeneity introduced by S substitution for Se, Adv. Quantum Technol. 6, 2300034 (2023).
- G. Tomassucci, L. Tortora, G. Pugliese, F. Stramaglia, L. Simonelli, C. Marini, K. Terashima, T. Wakita, S. Ayukawa, T. Yokoya, K. Kudo, M. Nohara, T. Mizokawa, and N. L. Saini, Temperature dependent local inhomogeneity and magnetic moments of ()OHFeSe superconductors, Phys. Chem. Chem. Phys. 25, 6684 (2023).
- M. M. Traum, G. Margaritondo, N. V. Smith, J. E. Rowe, and F. J. DiSalvo, : Semiconductor, semimetal, or excitonic insulator, Phys. Rev. B 17, 1836 (1978).
- M. Holt, P. Zschack, H. Hong, M. Y. Chou, and T. C. Chiang, X-ray studies of phonon softening in , Phys. Rev. Lett. 86, 3799 (2001).
- F. Weber, S. Rosenkranz, J. P. Castellan, R. Osborn, G. Karapetrov, R. Hott, R. Heid, K. P. Bohnen, and A. Alatas, Electron-phonon coupling and the soft phonon mode in , Phys. Rev. Lett. 107, 266401 (2011).
- H. Hughes, Structural distortion in and related materials-a possible Jahn-Teller effect? J. Phys. C 10, L319 (1977).
- M. Porer, U. Leierseder, J. Menard, H. Dachraoui, L. Mouchliadis, I. Perakis, U. Heinzmann, J. Demsar, K. Rossnagel, and R. Huber, Non-thermal separation of electronic and structural orders in a persisting charge density wave, Nat. Mater. 13, 857 (2014).
- A. Kogar, M. Rak, S. Vig, A. Husain, F. Flicker, Y. Joe, L. Venema, G. MacDougall, T. Chiang, E. Fradkin, J. van Wezel, and P. Abbamonte, Signatures of exciton condensation in a transition metal dichalcogenide, Science 358, 1314 (2017).
- S. Mathias, S. Eich, J. Urbancic, S. Michael, A. Carr, S. Emmerich, A. Stange, T. Popmintchev, T. Rohwer, M. Wiesenmayer, A. Ruffing, S. Jakobs, S. Hellmann, P. Matyba, C. Chen, L. Kipp, M. Bauer, H. C. Kapteyn, H. C. Schneider, K. Rossnagel, et al., Self-amplified photo-induced gap quenching in a correlated electron material, Nat. Commun. 7, 12902 (2016).
- E. Morosan, H. Zandbergen, B. Dennis, J. Bos, Y. Onose, T. Klimczuk, A. Ramirez, N. Ong, and R. Cava, Superconductivity in , Nat. Phys. 2, 544 (2006).
- S. Lee, T. B. Park, J. Kim, S. G. Jung, W. K. Seong, N. Hur, Y. Luo, D. Y. Kim, and T. Park, Tuning the charge density wave quantum critical point and the appearance of superconductivity in , Phys. Rev. Res. 3, 033097 (2021).
- S. Kitou, A. Nakano, S. Kobayashi, K. Sugawara, N. Katayama, N. Maejima, A. Machida, T. Watanuki, K. Ichimura, S. Tanda, T. Nakamura, and H. Sawa, Effect of Cu intercalation and pressure on excitonic interaction in 1T-, Phys. Rev. B 99, 104109 (2019).
- Y. Liu, D. F. Shao, L. J. Li, W. J. Lu, X. D. Zhu, P. Tong, R. C. Xiao, L. S. Ling, C. Y. Xi, L. Pi, H. F. Tian, H. X. Yang, J. Q. Li, W. H. Song, X. B. Zhu, and Y. P. Sun, Nature of charge density waves and superconductivity in 1T-, Phys. Rev. B 94, 045131 (2016).
- H. Luo, W. Xie, J. Tao, I. Pletikosic, T. Valla, G. Sahasrabudhe, G. Osterhoudt, E. Sutton, K. Burch, E. Seibel, J. W. Krizan, Y. Zhu, and R. J. Cava, Differences in chemical doping matter: Superconductivity in but not in , Chem. Mater. 28, 1927 (2016).
- E. Morosan, K. E. Wagner, L. L. Zhao, Y. Hor, A. J. Williams, J. Tao, Y. Zhu, and R. J. Cava, Multiple electronic transitions and superconductivity in , Phys. Rev. B 81, 094524 (2010).
- A. Zunger and A. J. Freeman, Band structure and lattice instability of , Phys. Rev. B 17, 1839 (1978).
- T. Kaneko, Y. Ohta, and S. Yunoki, Exciton-phonon cooperative mechanism of the triple-q charge-density-wave and antiferroelectric electron polarization in , Phys. Rev. B 97, 155131 (2018).
- S. Kitou, T. Hasegawa, A. Nakano, N. Katayama, S. Tsutsui, and H. Sawa, Intercalated Cu ion dynamics in the two-dimensional layered compound , Phys. Rev. B 101, 094108 (2020).
- J. F. Zhao, H. W. Ou, G. Wu, B. P. Xie, Y. Zhang, D. W. Shen, J. Wei, L. X. Yang, J. K. Dong, M. Arita, H. Namatame, M. Taniguchi, X. H. Chen, and D. L. Feng, Evolution of the electronic structure of 1T-, Phys. Rev. Lett. 99, 146401 (2007).
- J. Jeong, J. Jeong, H. Noh, S. B. Kim, and H.-D. Kim, Electronic structure study of Cu-doped 1T- by angle-resolved photoemission spectroscopy, Physica C 470, S648 (2010).
- D. Qian, D. Hsieh, L. Wray, Y. Xia, R. J. Cava, E. Morosan, and M. Z. Hasan, Evolution of low-lying states in a doped CDW superconductor , Phys. B: Condens. Matter 403, 1002 (2008).
- M. Bendele, A. Barinov, B. Joseph, D. Innocenti, A. Iadecola, A. Bianconi, H. Takeya, Y. Mizuguchi, Y. Takano, T. Noji, T. Hatakeda, Y. Koike, M. Horio, A. Fujimori, D. Ootsuki, T. Mizokawa, and N. L. Saini, Spectromicroscopy of electronic phase separation in superconductor, Sci. Rep. 4, 5592 (2014).
- T. Mizokawa, M. Bendele, A. Barinov, A. Iadecola, B. Joseph, T. Noji, Y. Koike, and N. L Saini, Mesoscopic stripes in antiferromagnetic Fe chalcogenide probed by scanning photoelectron spectromicroscopy, J. Phys. Soc. Jpn. 85, 033702 (2016).
- T. Mizokawa, A. Barinov, V. Kandyba, A. Giampietri, R. Matsumoto, Y. Okamoto, K. Takubo, K. Miyamoto, T. Okuda, S. Pyon, H. Ishii, K. Kudo, M. Nohara, and N. L. Saini, Domain dependent Fermi arcs observed in a striped phase dichalcogenide, Adv. Quantum Tech. 5, 2200029 (2022).
- T. Mizokawa, G. Tomassucci, M. Hattori, F. Minati, L. Tortora, A. Barinov, Z. Wang, J. X. Yin, and N. L. Saini, Electronic inhomogeneity in Cs- and Sb-terminated surfaces of probed by scanning photoemission spectromicroscopy, Phys. Rev. B 112, 075106 (2025).
- T. Sugimoto, E. Paris, K. Terashima, A. Barinov, A. Giampietri, T. Wakita, T. Yokoya, J. Kajitani, R. Higashinaka, T. D. Matsuda, T. Aoki, and N. L. Saini, Inhomogeneous charge distribution in a self-doped superconductor, Phys. Rev. B 100, 064520 (2019).
- T. Sugimoto, E. Paris, T. Wakita, K. Terashima, T. Yokoya, A. Barinov, J. Kajitani, R. Higashinaka, T. D. Matsuda, Y. Aoki, T. Mizokawa, and N. L. Saini, Metallic phase in stoichiometric revealed by space resolved ARPES, Sci. Rep. 8, 2011 (2018).
- F. Minati, G. Tomassucci, M. Hattori, Y. Fujita, M. Nagao, L. Tortora, A. Barinov, M. Kpciuszynski, G. Campi, L. Boeri, T. Mizokawa, and N. L. Saini, Intrinsic electronic structure and inhomogeneity of high-entropy layered superconductor, Inorg. Chem. 64, 11260 (2025).
- A. Titov, A. Merentsov, A. Kar'kin, A. Titov, and V. Fedorenko, Structure and properties of the intercalation compound , Phys. Solid State 51, 230 (2009).
- S. Kitou, S. Kobayashi, T. Kaneko, N. Katayama, S. Yunoki, T. Nakamura, and H. Sawa, Honeycomb lattice type charge density wave associated with interlayer Cu ions ordering in 1T-, Phys. Rev. B 99, 081111(R) (2019).
- K. Momma and F. Izumi, VESTA3 for three-dimensional visualization of crystal, volumetric and morphology data, J. Appl. Crystallogr. 44, 1272 (2011).
- P. Dudin, P. Lacovig, C. Fava, E. Nicolini, A. Bianco, G. Cautero, and A. Barinov, Angle-resolved photoemission spectroscopy and imaging with a submicrometre probe at the SPECTROMICROSCOPY-3.2L beamline of Elettra, J. Synchrotron Radiat. 17, 445 (2010).
- P. Blaha, K. Schwarz, F. Tran, R. Laskowski, G. K. H. Madsen, and L. D. Marks, WIEN2k: An APW lo program for calculating the properties of solids, J. Chem. Phys. 152, 074101 (2020).
- J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
- M. Huber, Y. Lin, G. Marini, L. Moreschini, C. Jozwiak, A. Bostwick, M. Calandra, and A. Lanzara, Ultrafast creation of a light-induced semimetallic state in strongly excited 1T-, Sci. Adv. 10, eadl4481 (2024).
- R. Bianco, M. Calandra, and F. Mauri, Electronic and vibrational properties of in the charge-density-wave phase from first principles, Phys. Rev. B 92, 094107 (2015).
- H. J. Monkhorst and J. D. Pack, Special points for Brillouin-zone integrations, Phys. Rev. B 13, 5188 (1976).
- O. Rubel, J. B. Moussy, P. Foulquier, and V. Brouet, Band unfolding with a general transformation matrix: From code implementation to interpretation of photoemission spectra, Comput. Phys. Commun. 291, 108800 (2023).
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/dg1f-hm99 for additional spectromicroscopy and space resolved ARPES data.
- M. Spera, A. Scarfato, E. Giannini, and C. Renner, Energy-dependent spatial texturing of charge order in 1T-, Phys. Rev. B 99, 155133 (2019).
- A. M. Novello, M. Spera, A. Scarfato, A. Ubaldini, E. Giannini, D. R. Bowler, and C. Renner, Stripe and short range order in the charge density wave of 1T-, Phys. Rev. Lett. 118, 017002 (2017).
- S. Yan, D. Iaia, E. Morosan, E. Fradkin, P. Abbamonte, and V. Madhavan, Influence of domain walls in the incommensurate charge density wave state of Cu intercalated 1T-, Phys. Rev. Lett. 118, 106405 (2017).
- H. Cercellier, C. Monney, F. Clerc, C. Battaglia, L. Despont, M. G. Garnier, H. Beck, P. Aebi, L. Patthey, H. Berger, and L. Forro, Evidence for an excitonic insulator phase in 1T-, Phys. Rev. Lett. 99, 146403 (2007).
- R. A. Jishi and H. M. Alyahyaei, Electronic structure of superconducting copper intercalated transition metal dichalcogenides: First-principles calculations, Phys. Rev. B 78, 144516 (2008).
- C. Chen, B. Singh, H. Lin, and V. M. Pereira, Reproduction of the charge density wave phase diagram in 1T- exposes its excitonic character, Phys. Rev. Lett. 121, 226602 (2018).