- Letter
- Open Access
Frustration-driven correlated parent states in the spinel superconductor
Phys. Rev. Research 8, L012032 – Published 4 February, 2026
DOI: https://doi.org/10.1103/q3xq-6p5f
Abstract
Geometrically frustrated transition-metal oxides provide fertile ground for the emergence of novel quantum states. In the spinel superconductor (superconducting critical temperature , formal system), we uncover a prominent dispersion kink near the Fermi energy accompanied by negative thermal expansion below a characteristic temperature . We propose that charge frustration in the pyrochlore lattice leads to a degenerate electronic arrangement on sites, giving rise to strong intersite Coulomb interactions below . Within this framework, negative thermal expansion arises from the Coulomb repulsion of electrons, while the prominent kink reflects reduced screening due to enhanced correlations. These findings open up promising avenues for exploring exotic correlated states in frustrated pyrochlore lattices, which are situated near the Mott state.
Physics Subject Headings (PhySH)
Article Text
Supplemental Material
References (67)
- E. J. W. Verwey, Electronic conduction of magnetite and its transition point at low temperatures, Nature (London) 144, 327 (1939).
- P. Anderson, Ordering and antiferromagnetism in ferrites, Phys. Rev. 102, 1008 (1956).
- S.-H. Lee, C. Broholm, T. H. Kim, W. Ratcliff II, and S-W. Cheong, Local spin resonance and spin-Peierls-like phase transition in a geometrically frustrated antiferromagnet, Phys. Rev. Lett. 84, 3718 (2000).
- T. He, X. Zhang, Y. Liu, X. Dai, L. Wang, and G. Liu, Potential antiferromagnetic Weyl nodal line state in material, Phys. Rev. B 104, 045143 (2021).
- S. Kondo, D. C. Johnston, C. A. Swenson, F. Borsa, A. V. Mahajan, L. L. Miller, T. Gu, A. I. Goldman, and M. B. Maple, : A heavy fermion transition metal oxide, Phys. Rev. Lett. 78, 3729 (1997).
- C. Urano, M. Nohara, S. Kondo, F. Sakai, H. Takagi, T. Shiraki, and T. Okubo, Spinel as a heavy-mass Fermi liquid: Anomalous transport and role of geometrical frustration, Phys. Rev. Lett. 85, 1052 (2000).
- Y. Shimizu, H. Takeda, M. Tanaka, M. Itoh, S. Niitaka, and H. Takagi, An orbital-selective spin liquid in a frustrated heavy fermion spinel , Nat. Commun. 3, 981 (2012).
- U. Niemann, Y.-M. Wu, R. Oka, D. Hirai, Y. Wang, Y. E. Suyolcu, M. Kim, P. A. van Aken, and H. Takagi, Crystallization of heavy fermion via epitaxial strain in spinel thin film, Proc. Natl Acad. Sci. USA 120, e2215722120 (2023).
- K. Matsuno, T. Katsufuji, S. Mori, Y. Moritomo, A. Machida, E. Nishibori, M. Tanaka, M. Sakata, N. Yamamoto, and H. Takagi, Charge ordering in the geometrically frustrated spinel , J. Phys. Soc. Jpn. 70, 1456 (2001).
- D. C. Johnston, H. Prakash, W. H. Zachariasen, and R. Viswanathan, High-temperature superconductivity in the Li-Ti-O ternary system, Mat. Res. Bull 8, 777 (1973).
- H. Xue, L. Wang, Z. Wang, G. Zhang, W. Peng, S. Wu, C.-L. Gao, Z. An, Y. Chen, and W. Li, Fourfold symmetric superconductivity in spinel oxide (001) thin films, ACS Nano 16, 19464 (2022).
- W. Hu, Z. Feng, B.-C. Gong, G. He, D. Li, M. Qin, Y. Shi, Q. Li, Q. Zhang, J. Yuan, B. Zhu, K. Liu, T. Xiang, L. Gu, F. Zhou, X. Dong, Z. Zhao, and K. Jin, Emergent superconductivity in single-crystalline films via structural engineering, Phys. Rev. B 101, 220510 (R) (2020).
- Y. Okamoto, S. Niitaka, M. Uchida, T. Waki, M. Takigawa, Y. Nakatsu, A. Sekiyama, S. Suga, R. Arita, and H. Takagi, Band Jahn-Teller instability and formation of valence bond solid in a mixed-valent spinel oxide , Phys. Rev. Lett. 101, 086404 (2008).
- M. Schmidt, W. Ratcliff II, P. G. Radaelli, K. Refson, N. M. Harrison, and S. W. Cheong, Spin singlet formation in : Evidence of a helical dimerization pattern, Phys. Rev. Lett. 92, 056402 (2004).
- J. G. Azadani, W. Jiang, J-P. Wang, and T. Low, Ferromagnetic phase of the spinel compound and its spintronics properties, Phys. Rev. B 102, 155144 (2020).
- K. Tanaka, W. S. Lee, D. H. Lu, A. Fujimori, T. Fujii, Risdiana, I. Terasaki, D. J. Scalapino, T. P. Devereaux, Z. Hussain, and Z.-X. Shen, Distinct Fermi-momentum-dependent energy gaps in deeply underdoped Bi2212, Science 314, 1910 (2006).
- K. Nakayama, Y. Miyata, G. N. Phan, T. Sato, Y. Tanabe, T. Urata, K. Tanigaki, and T. Takahashi, Reconstruction of band structure induced by electronic nematicity in an FeSe superconductor, Phys. Rev. Lett. 113, 237001 (2014).
- V. Brouet, W. L. Yang, X. J. Zhou, Z. Hussain, N. Ru, K. Y. Shin, I. R. Fisher, and Z. X. Shen, Fermi surface reconstruction in the CDW state of observed by photoemission, Phys. Rev. Lett. 93, 126405 (2004).
- V. Anisimov, M. A. Korotin, M. Zölfl, T. Pruschke, K. Le Hur, and T. M. Rice, Electronic structure of the heavy fermion metal , Phys. Rev. Lett. 83, 364 (1999).
- Y. Okada, Y. Ando, R. Shimizu, E. Minamitani, S. Shiraki, S. Watanabe, and T. Hitosugi, Scanning tunnelling spectroscopy of superconductivity on surfaces of thin films, Nat. Commun. 8, 15975 (2017).
- K. Jin, G. He, X. Zhang, S. Maruyama, S. Yasui, R. Suchoski, J. Shin, Y. Jiang, H. S. Yu, J. Yuan, L. Shan, F. V. Kusmartsev, R. L. Greene, and I. Takeuchi, Anomalous magnetoresistance in the spinel superconductor , Nat. Commun. 6, 7183 (2015).
- Z. Wei, Q. Li, B.-C. Gong, X. Wei, W. Hu, Z. Ni, G. He, M. Qin, A. Kusmartseva, F. V. Kusmartsev, J. Yuan, B. Zhu, Q. Chen, J.-H. Chen, K. Liu, and K. Jin, Two superconductor-insulator phase transitions in the spinel oxide induced by ionic liquid gating, Phys. Rev. B 103, L140501 (2021).
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/q3xq-6p5f for experimental and theoretical methods, sample characterization, extended ARPES and XRD data, and theoretical considerations, which includes Refs. [51, 52, 53, 54, 55, 56, 57, 58, 59, 60, 61, 62, 63, 64, 65, 66, 67].
- H. Luo, Q. Gao, H. Liu, Y. Gu, D. Wu, C. Yi, J. Jia, S. Wu, X. Luo, Y. Xu, L. Zhao, Q. Wang, H. Mao, G. Liu, Z. Zhu, Y. Shi, K. Jiang, J. Hu, Z. Xu, and X. J. Xhou, Electronic nature of charge density wave and electron-phonon coupling in Kagome superconductor , Nat. Commun. 13, 273 (2022).
- L. Ye, M. Kang, J. Liu, F. Von Cube, C. R. Wicker, Y. Suzuki, C. Jozwiak, A. Bostwick, E. Rotenberg, D. C. Bell, L. Fu, R. Comin, and J. G. Checkelsky, Massive Dirac fermions in a ferromagnetic Kagome metal, Nature (London) 555, 638 (2018).
- M. Kang, et al., Dirac fermions and flat bands in the ideal Kagome metal FeSn, Nat. Mater. 19, 163 (2020).
- Z. Hasan, et al., Unconventional polaronic ground state in superconducting , arXiv:2505.09762.
- Min-Yi-Nan Lei, X. Wang, P.-Y. Zheng, X.-X. Wang, X.-Y. Chen, Z.-H. Chen, Y.-N. Hu, N. Guo, Z.-P. Yin, T. Zhang, R. Peng, H. Xu, and D. Feng, Anisotropic band renormalization and nodeless gap of spinel superconductor, Phys. Rev. B 112, 045105 (2025).
- A. Damascelli, Z. Hussain, and Z-X. Shen, Angle-resolved photoemission studies of the cuprate superconductors, Rev. Mod. Phys. 75, 473 (2003).
- T. L. Yu, M. Xu, W. T. Yang, Y. H. Song, C. H. P. Wen, Q. Yao, X. Lou, T. Zhang, W. Li, X. Y. Wei, J. K. Bao, G. H. Cao, P. Dudin, J. D. Denlinger, V. N. Strocov, R. Peng, H. C. Xu, and D. L. Feng, Strong band renormalization and emergent ferromagnetism induced by electron-antiferromagnetic-magnon coupling, Nat. Commun. 13, 6560 (2022).
- In the case of pure aluminum (Al), for example, assuming the temperature-independent Eliashberg function, experimentally obtained λ(T) is reproduced by this method. See J. Jiang, K. Shimada, H. Hayashi, H. Iwasawa, Y. Aiura, H. Namatame, and M. Taniguchi, Coupling parameters of many-body interactions for the Al(100) surface state: A high-resolution angle-resolved photoemission spectroscopy, Phys. Rev. B 84, 155124 (2011).
- J. Chen, L. Hu, J. Deng, and X. Xing, Negative thermal expansion in functional materials: Controllable thermal expansion by chemical modifications, Chem. Soc. Rev. 44, 3522 (2015).
- L. Hu, Y. Zhu, Y.-W. Fang, M. Fukuda, T. Nishikubo, Z. Pan, Y. Sakai, S. Kawaguchi, H. Das, A. Machida, T. Watanuki, S. Mori, K. Takenaka, and M. Azuma, Origin and absence of giant negative thermal expansion in reduced and oxidized , Chem. Mater. 33, 7665 (2021).
- E. Pachound, J. Cumby, C. T. Lithgow, and J. P. Attfield, Charge order and negative thermal expansion in , J. Am. Chem. Soc. 140, 636 (2018).
- L. Balents, Spin liquids in frustrated magnets, Nature (London) 464, 199 (2010).
- A. P. Ramirez, C. L. Broholm, R. J. Cava, and G. R. Kowach, Geometrical frustration, spin ice and negative thermal expansion–The physics of underconstraint, Physica B 280, 290 (2000).
- N. Tang, Y. Gritsenko, K. Kimura, S. Bhattacharjee, A. Sakai, M. Fu, H. Takeda, H. Man, K. Sugawara, Y. Matsumoto, Y. Shimura, J. Wen, C. Broholm, H. Sawa, M. Takigawa, T. Sakakibara, S. Zherlitsyn, J. Wosnitza, R. Moessner, and S. Nakatsuji, Spin-orbital liquid state and liquid-gas metamagnetic transition on a pyrochlore lattice, Nat. Phys. 19, 92 (2023).
- S. Kitani, M. Tachibana, N. Taira, and H. Kawaji, Thermal study of the interplay between spin and lattice in and , Phys. Rev. B 87, 064402 (2013).
- Y. Shimura, A. Wörl, M. Sundermann, S. Tsuda, D. T. Adroja, A. Bhattacharyya, A. M. Strydom, A. D. Hillier, F. L. Pratt, A. Gloskovskii, A. Severing, T. Onimaru, P. Gegenwart, and T. Takabatake, Antiferromagnetic correlations in strongly valence fluctuating CeIrSn, Phys. Rev. Lett. 126, 217202 (2021).
- R. Zuyher and M. Kulic, Renormalization of the electron-phonon interaction by strong electronic correlations in high- superconductors, Phys. Rev. B 53, 2850 (1996).
- G. Ernst, C. Broholm, G. R. Kowach, and A. P. Ramirez, Phonon density of states and negative thermal expansion in , Nature (London) 396, 147 (1998).
- T. A. Mary, J. S. O. Evans, T. Vogt, and A. W. Sleight, Negative thermal expansion from 0.3 to 1050 Kelvin in , Science 272, 90 (1996).
- S. Backes, Y. Nomura, R. Arita, and H. Shinaoka, Ab initio study on heavy-fermion behavior in : Role of Hund's coupling and stability, Phys. Rev. B 111, L041102 (2025).
- M. Grundner, F. B. Kugler, O. Parcollet, U. Schollwöck, A. Georges, and A. Hampel, : Hund-assisted orbital-selective Mottness, Phys. Rev. B 112, L041106 (2025).
- D. Oh, et al., Hund flat band in a frustrated spinel oxide, arXiv:2502.07234.
- J. Graf, G-H. Gweon, K. McElroy, S. Y. Zhou, C. Jozwiak, E. Rotenberg, A. Bill, T. Sasagawa, H. Eisaki, S. Uchida, H. Takagi, D.-H. Lee, and A. Lanzara, Universal high energy anomaly in the angle-resolved photoemission spectra of high temperature superconductors: Possible evidence of spinon and holon branches, Phys. Rev. Lett. 98, 067004 (2007).
- H. Iwasawa, Y. Yoshida, I. Hase, K. Shimada, H. Namatame, M. Taniguchi, and Y. Aiura, High-energy anomaly in the band dispersion of the ruthenate superconductor, Phys. Rev. Lett. 109, 066404 (2012).
- S. Aizaki, T. Yoshida, K. Yoshimatsu, M. Takizawa, M. Minohara, S. Ideta, A. Fujimori, K. Gputa, P. Mahadevan, K. Horiba, H. Kumigashira, and M. Oshima, Self-energy on the low- to high-energy electronic structure of correlated metal , Phys. Rev. Lett. 109, 056401 (2012).
- Y. Fujisawa, A. Krishnadas, T. Nakamura, C.-H. Hsu, B. Smith, M. P. Almanza, H. Hiyane, G. Chang, Y. Nagai, T. Machida, and Y. Okada, Imaging Josephson vortices on curved junctions, Phys. Rev. B 110, 224511 (2024).
- Y. Fujisawa, A. Krishnadas, C.-H. Hsu, B. R. M. Smith, M. P. Almanza, Y. Obata, D. van Dinter, G. Chang, Y. Nagai, T. Machida, and Y. Okada, Visualizing magnetic field-induced rotational electronic symmetry breaking in a spinel oxide superconductor, arXiv:2306.06711.
- Y. Fujisawa, M. Pardo-Almanza, C. H. Hsu, A. Mohamed, K. Yamagami, A. Krishnadas, G. Chang, F.-C. Chuang, K. H. Khoo, J. Zang, A. Soumyanarayanan, and Y. Okada, Widely tunable Berry curvature in the magnetic semimetal , Adv. Mat. 35, 2207121 (2023).
- T. Kawamoto, A. Krishnadas, M. Pardo-Almanza, Y. Fujisawa, G. Chang, T. Harada, and Y. Okada, Visualization of robust two-dimensional bulk states with suppressed surface state on epitaxial thin films with bipolar surfaces, Phys. Rev. Mat. 7, 024001 (2023).
- G. Kresse and J. Hafner, Ab initio molecular dynamics for liquid metals, Phys. Rev. B 47, 558 (1993).
- G. Kresse and J. Furthmüller, Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set, Phys. Rev. B 54, 11169 (1996).
- G. Kresse and D. Joubert, From ultrasoft pseudopotentials to the projector augmented-wave method, Phys. Rev. B 59, 1758 (1999).
- J. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
- H. J. Monkhorst and J. D. Pack, Special points for Brillouin-zone integrations, Phys. Rev. B 13, 5188 (1976).
- P. Giannozzi, O. Andreussi, T. Brumme, O. Bunau, M. Buongiorno Nardelli, M. Calandra, R. Car, C. Cavazzoni, D. Ceresoli, and M. Cococcioni, Advanced capabilities for materials modelling with quantum espresso, J. Phys.: Condens. Matter 29, 465901 (2017).
- J. Noffsinger, F. Giustino, B. D. Malone, C.-H. Park, S. G. Louie, and M. L. Cohen, EPW: A program for calculating the electron-phonon coupling using maximally localized Wannier functions, Comput. Phys. Commun. 181, 2140 (2010).
- S. Poncé, E. Margine, C. Verdi, and F. Giustino, EPW: Electron-phonon coupling, transport and superconducting properties using maximally localized Wannier functions, Comput. Phys. Commun. 209, 116 (2016).
- H. X. Geng, A. F. Dong, G. C. Che, W. W. Huang, S. L. Jia, and Z. X. Zhai, Investigations on preparation, upper critical field and low temperature thermal expansion of superconductor, Physica C 432, 53 (2005).
- T. Harada, K. Fujiwara, and A. Tsukazaki, Highly conductive ultrathin films for transparent electrodes, APL Mat. 6, 046107 (2018).
- J. Huang, et al., Observation of flat bands and Dirac cones in a pyrochlore lattice superconductor, npj Quantum Mater. 9, 71 (2024).
- J. Huang, L. Chen, Y. Huang, C. Setty, B. Gao, Y. Shi, Z. Liu, Y. Zhang, T. Yilmaz, E. Vescovo, M. Hashimoto, D. Lu, B. I. Yakobson, P. Dai, J.-H. Chu, Q. Si, and M. Yi, Non-Fermi liquid behavior in a correlated flat-band pyrochlore lattice, Nat. Phys. 20, 603 (2024).
- G. Grimvall, The Electron-Phonon Interaction in Metals (North-Holland, Amsterdam, 1981).
- N. Mannella, W. L. Yang, X. J. Zhou, H. Zheng, J. F. Mitchell, J. Zaanen, T. P. Devereaux, N. Nagaosa, Z. Hussain, and Z.-X. Shen, Nodal quasiparticle in pseudogapped colossal magnetoresistive manganites, Nature (London) 438, 474 (2005).
- D. I. Khomskii and T. Mizokawa, Orbitally induced Peierls state in spinels, Phys. Rev. Lett. 94, 156402 (2015).