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Magnetic-field-driven phase switching in the antiferromagnetic Mott insulator Ca3(Ru0.99Ti0.01)2O7

Ksenia S. Rabinovich1,*, Tim Priessnitz1,*, Nils Gross1,*, George Jackeli1,2, Maximilian J. Krautloher1, Pascal Reiss1, Eberhard J. Goering1, Jurgen H. Smet1, Bernhard Keimer1 et al.

Alexander V. Boris1,†

  • *These authors contributed equally to this work.
  • †Contact author: A.Boris@fkf.mpg.de

Phys. Rev. B 114, 185134 – Published 30 September, 2026

DOI: https://doi.org/10.1103/z696-28zn

Abstract

A bandwidth-controlled antiferromagnetic Mott-insulating phase in Ca3(Ru1−xTix)2O7 is realized through isovalent substitution of the Ru site. For a dilute substitution with only 1% Ti, the Mott insulator ground state remains nearly degenerate with the ground state of pristine Ca3Ru2O7, where the Ru moments are ferromagnetically aligned within the metallic RuO2 bilayers, which are stacked in an antiferromagnetic fashion. The exceptionally shallow free-energy landscape of this doped compound arises from intertwined electron–electron and electron–lattice interactions. This makes its magnetic and transport properties highly sensitive to external perturbations. We systematically investigated magnetic-field-induced phase switching in Ca3(Ru0.99Ti0.01)2O7 to explore its magnetic H−T phase diagram. With the field applied along the easy b axis, parallel to the antiferromagnetic moments, the magnetization exhibits a first-order spin-flop transition at ≈6T, indicating reorientation of the Ru moments perpendicular to the field. The transition is accompanied by a decrease in the electrical resistance, but the spin-flop phase remains insulating. Above 10.5T, all Ru moments align with the b axis, resulting in a forced ferromagnetic metallic phase. In contrast, neither spin-flop nor forced ferromagnetic phases are observed up to 14T when the field is applied along the a axis. While the electronic kinetic energy and the electron–lattice coupling contribute to the free-energy balance of this system, the resulting H−T phase diagram is remarkably simple and closely resembles that of a canonical anisotropic antiferromagnet, albeit with substantially renormalized critical fields.

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References (40)

  1. G. Cao, C. Alexander, S. McCall, J. Crow, and R. Guertin, From antiferromagnetic insulator to ferromagnetic metal: A brief review of the layered ruthenates, Mater. Sci. Eng. B 63, 76 (1999).
  2. G. Cao, S. McCall, J. E. Crow, and R. P. Guertin, Observation of a metallic antiferromagnetic phase and metal to nonmetal transition in Ca3Ru2O7, Phys. Rev. Lett. 78, 1751 (1997).
  3. S.-I. Ikeda, Y. Maeno, S. Nakatsuji, M. Kosaka, and Y. Uwatoko, Ground state in Sr3Ru2O7: Fermi liquid close to a ferromagnetic instability, Phys. Rev. B 62, R6089 (2000).
  4. Y. Maeno, T. M. Rice, and M. Sigrist, The intriguing superconductivity of strontium ruthenate, Phys. Today 54(1), 42 (2001).
  5. G. Cuono, R. M. Sattigeri, J. Skolimowski, and C. Autieri, Orbital-selective altermagnetism and correlation-enhanced spin-splitting in strongly-correlated transition metal oxides, J. Magn. Magn. Mater. 586, 171163 (2023).
  6. A. León, C. Autieri, T. Brumme, and J. W. González, Hybrid d/p-wave altermagnetism in Ca3Ru2O7 and strain-controlled spin splitting, npj Quantum Mater. 10, 98 (2025).
  7. C. S. Snow, S. L. Cooper, G. Cao, J. E. Crow, H. Fukazawa, S. Nakatsuji, and Y. Maeno, Pressure-tuned collapse of the Mott-like state in Can+1RunO3n+1 (n = 1, 2): Raman spectroscopic studies, Phys. Rev. Lett. 89, 226401 (2002).
  8. J. Bertinshaw, N. Gurung, P. Jorba, H. Liu, M. Schmid, D. T. Mantadakis, M. Daghofer, M. Krautloher, A. Jain, G. H. Ryu, O. Fabelo, P. Hansmann, G. Khaliullin, C. Pfleiderer, B. Keimer, and B. J. Kim, Unique crystal structure of Ca2RuO4 in the current stabilized semimetallic state, Phys. Rev. Lett. 123, 137204 (2019).
  9. J. Zhang, A. S. McLeod, Q. Han, X. Chen, H. A. Bechtel, Z. Yao, S. N. G. Corder, T. Ciavatti, T. H. Tao, M. Aronson, G. L. Carr, M. C. Martin, C. Sow, S. Yonezawa, F. Nakamura, I. Terasaki, D. N. Basov, A. J. Millis, Y. Maeno, and M. Liu, Nano-resolved current-induced insulator-metal transition in the Mott insulator Ca2RuO4, Phys. Rev. X 9, 011032 (2019).
  10. C. T. Suen, I. Marković, M. Zonno, N. Heinsdorf, S. Zhdanovich, N. H. Jo, M. Schmid, P. Hansmann, P. Puphal, K. Fürsich, et al., Electronic response of a Mott insulator at a current-induced insulator-to-metal transition, Nat. Phys. 20, 1757 (2024).
  11. K. S. Rabinovich, A. N. Yaresko, R. D. Dawson, M. J. Krautloher, T. Priessnitz, Y. Mathis, A. Kirilyuk, B. Keimer, and A. V. Boris, Optically driven dynamics of a Mott insulator‐to‐metal transition, Adv. Funct. Mater. 35, 2416597 (2025).
  12. W. Bao, Z. Q. Mao, Z. Qu, and J. W. Lynn, Spin valve effect and magnetoresistivity in single crystalline Ca3Ru2O7, Phys. Rev. Lett. 100, 247203 (2008).
  13. B. Bohnenbuck, I. Zegkinoglou, J. Strempfer, C. Schüßler-Langeheine, C. S. Nelson, P. Leininger, H.-H. Wu, E. Schierle, J. C. Lang, G. Srajer, S. I. Ikeda, Y. Yoshida, K. Iwata, S. Katano, N. Kikugawa, and B. Keimer, Magnetic structure and orbital state of Ca3Ru2O7 investigated by resonant x-ray diffraction, Phys. Rev. B 77, 224412 (2008).
  14. D. Sokolov, N. Kikugawa, T. Helm, H. Borrmann, U. Burkhardt, R. Cubitt, J. White, E. Ressouche, M. Bleuel, K. Kummer, et al., Metamagnetic texture in a polar antiferromagnet, Nat. Phys. 15, 671 (2019).
  15. I. Marković, M. D. Watson, O. J. Clark, F. Mazzola, E. A. Morales, C. A. Hooley, H. Rosner, C. M. Polley, T. Balasubramanian, S. Mukherjee, et al., Electronically driven spin-reorientation transition of the correlated polar metal Ca3Ru2O7, Proc. Natl. Acad. Sci. USA 117, 15524 (2020).
  16. Q. Faure, C. D. Dashwood, C. V. Colin, R. D. Johnson, E. Ressouche, G. B. G. Stenning, J. Spratt, D. F. McMorrow, and R. S. Perry, Magnetic structure and field dependence of the cycloid phase mediating the spin reorientation transition in Ca3Ru2O7, Phys. Rev. Res. 5, 013040 (2023).
  17. X. Ke, J. Peng, D. J. Singh, T. Hong, W. Tian, C. R. Dela Cruz, and Z. Q. Mao, Emergent electronic and magnetic state in Ca3Ru2O7 induced by Ti doping, Phys. Rev. B 84, 201102(R) (2011).
  18. S. Tsuda, N. Kikugawa, K. Sugii, S. Uji, S. Ueda, M. Nishio, and Y. Maeno, Mott transition extremely sensitive to impurities in Ca3Ru2O7 revealed by hard x-ray photoemission studies, Phys. Rev. B 87, 241107(R) (2013).
  19. M. Krautloher, Neutron scattering studies on layered ruthenates, Ph.D. thesis, Universität Stuttgart, 2018.
  20. S. Shrestha, M. Souri, C. J. Dietl, E. M. Pärschke, M. Krautloher, G. A. C. Ortiz, M. Minola, X. Shi, A. V. Boris, J. Hwang, et al., Tunable magnons of an antiferromagnetic Mott insulator via interfacial metal-insulator transitions, Nat. Commun. 16, 3592 (2025).
  21. V. Baltz, A. Manchon, M. Tsoi, T. Moriyama, T. Ono, and Y. Tserkovnyak, Antiferromagnetic spintronics, Rev. Mod. Phys. 90, 015005 (2018).
  22. O. Gomonay, V. Baltz, A. Brataas, and Y. Tserkovnyak, Antiferromagnetic spin textures and dynamics, Nat. Phys. 14, 213 (2018).
  23. N. O. Antropov, E. A. Kravtsov, M. V. Makarova, V. V. Proglyado, T. Keller, I. A. Subbotin, E. M. Pashaev, G. V. Prutskov, A. L. Vasiliev, Y. M. Chesnokov, N. G. Bebenin, M. A. Milyaev, V. V. Ustinov, B. Keimer, and Y. N. Khaydukov, Tunable spin-flop transition in artificial ferrimagnets, Phys. Rev. B 104, 054414 (2021).
  24. H. Chen, L. Liu, X. Zhou, Z. Meng, X. Wang, Z. Duan, G. Zhao, H. Yan, P. Qin, and Z. Liu, Emerging antiferromagnets for spintronics, Adv. Mater. 36, 2310379 (2024).
  25. J. Peng, J. Y. Liu, X. Gu, G. Zhou, W. Wang, J. Hu, F. M. Zhang, and X. S. Wu, Extremely large anisotropic transport caused by electronic phase separation in Ti-doped Ca3Ru2O7, J. Phys. D: Appl. Phys. 49, 245004 (2016).
  26. J. Peng, J. Y. Liu, J. Hu, Z. Q. Mao, F. M. Zhang, and X. S. Wu, Magnetic phase separation in double layer ruthenates Ca3(Ru1−xTix)2O7, Sci. Rep. 6, 19462 (2016).
  27. M. Zhu, J. Peng, T. Zou, K. Prokes, S. D. Mahanti, T. Hong, Z. Q. Mao, G. Q. Liu, and X. Ke, Colossal magnetoresistance in a Mott insulator via magnetic field-driven insulator-metal transition, Phys. Rev. Lett. 116, 216401 (2016).
  28. F. Nakamura, M. Sakaki, Y. Yamanaka, S. Tamaru, T. Suzuki, and Y. Maeno, Electric-field-induced metal maintained by current of the Mott insulator Ca2RuO4, Sci. Rep. 3, 2536 (2013).
  29. R. Okazaki, Y. Nishina, Y. Yasui, F. Nakamura, T. Suzuki, and I. Terasaki, Current-induced gap suppression in the Mott insulator Ca2RuO4, J. Phys. Soc. Jpn. 82, 103702 (2013).
  30. P. Heller, Nuclear-magnetic-resonance studies of critical phenomena in MnF2. I. Time-average properties, Phys. Rev. 146, 403 (1966).
  31. Y. Shapira and S. Foner, Magnetic phase diagram of MnF2 from ultrasonic and differential magnetization measurements, Phys. Rev. B 1, 3083 (1970).
  32. J. Bertinshaw, M. L. Krautloher, L. Wang, H. Trepka, J. Porras, M. Hepting, S. Francoual, E. Ressouche, B. J. Kim, and B. Keimer, Extreme sensitivity to perturbation in Ti-doped Ca3Ru2O7 (unpublished).
  33. M. E. Fisher, Relation between the specific heat and susceptibility of an antiferromagnet, Philos. Mag. 7, 1731 (1962).
  34. M. J. Krautloher, J. Bertinshaw, J. Porras, D. G. Joshi, H. Trepka, M. Hepting, D. Adroja, H. Walker, A. Ivanov, M. Enderle, et al., Impurity induced localization of low-energy spin excitations in bilayer ruthenate Ca3Ru2O7 (unpublished).
  35. J. Bertinshaw, H. Suzuki, H. Takahashi, M. Krautloher, K. S. Rabinovich, G. Khaliullin, A. V. Boris, H. Gretarsson, and B. Keimer, The emergence of spin-orbit excitations in Ti-doped Ca3Ru2O7 (unpublished).
  36. A. R. King and H. Rohrer, Spin-flop bicritical point in MnF2, Phys. Rev. B 19, 5864 (1979).
  37. K. Aoyama and H. Kawamura, Spin-lattice-coupled order in Heisenberg antiferromagnets on the pyrochlore lattice, Phys. Rev. Lett. 116, 257201 (2016).
  38. J. SS and D. Bansal, Effect of spin-phonon coupling on phonons and magnons in the antiferromagnet NiO, Phys. Rev. B 111, 104306 (2025).
  39. Y. Tokura, Critical features of colossal magnetoresistive manganites, Rep. Prog. Phys. 69, 797 (2006).
  40. X. N. Lin, Z. X. Zhou, V. Durairaj, P. Schlottmann, and G. Cao, Colossal magnetoresistance by avoiding a ferromagnetic state in the Mott system Ca3Ru2O7, Phys. Rev. Lett. 95, 017203 (2005).

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